Urea holds promise as an alternative water-oxidation substrate in electrolytic cells.High-valence nickelbased spinel,especially after heteroatom doping,excels in urea oxidation reactions(UOR).However,traditional spine...Urea holds promise as an alternative water-oxidation substrate in electrolytic cells.High-valence nickelbased spinel,especially after heteroatom doping,excels in urea oxidation reactions(UOR).However,traditional spinel synthesis methods with prolonged high-temperature reactions lack kinetic precision,hindering the balance between controlled doping and highly active two-dimensional(2D)porous structures design.This significantly impedes the identification of electron configuration-dependent active sites in doped 2D nickel-based spinels.Herein,we present a microwave shock method for the preparation of 2D porous NiCo_(2)O_(4)spinel.Utilizing the transient on-off property of microwave pulses for precise heteroatom doping and 2D porous structural design,non-metal doping(boron,phosphorus,and sulfur)with distinct extranuclear electron disparities serves as straightforward examples for investigation.Precise tuning of lattice parameter reveals the impact of covalent bond strength on NiCo_(2)O_(4)structural stability.The introduced defect levels induce unpaired d-electrons in transition metals,enhancing the adsorption of electron-donating amino groups in urea molecules.Simultaneously,Bode plots confirm the impact mechanism of rapid electron migration caused by reduced band gaps on UOR activity.The prepared phosphorus-doped 2D porous NiCo_(2)O_(4),with optimal electron configuration control,outperforms most reported spinels.This controlled modification strategy advances understanding theoretical structure-activity mechanisms of high-performance 2D spinels in UOR.展开更多
Hydrogen evolution reaction(HER)and urea oxidation reaction(UOR)are key reactions of the watercycling associated catalytic process/device.The design of catalysts with a super-hydrophilic/aerophobic structure and optim...Hydrogen evolution reaction(HER)and urea oxidation reaction(UOR)are key reactions of the watercycling associated catalytic process/device.The design of catalysts with a super-hydrophilic/aerophobic structure and optimized electron distribution holds great promise.Here,we have designed a threedimensional(3D)hollow Ni/NiMoN hierarchical structure with arrayed-sheet surface based on a onepot hydrothermal route for efficient urea-assisted HER based on a simple hydrothermal process.The Ni/NiMoN catalyst exhibits super-hydrophilic/aerophobic properties with a small droplet contact angle of 6.07°and an underwater bubble contact angle of 155.7°,thus facilitating an escape of bubbles from the electrodes.Density functional theory calculations and X-ray photoelectron spectroscopy results indicate the optimized electronic structure at the interface of Ni and NiMoN,which can promote the adsorption/desorption of reactants and intermediates.The virtues combining with a large specific surface area endow Ni/NiMoN with efficient catalytic activity of low potentials of 25 mV for HER and 1.33 V for UOR at10 mA cm^(-2).The coupled HER and UOR system demonstrates a low cell voltage of 1.42 V at 10 mA cm^(-2),which is approximately 209 mV lower than water electrolysis.展开更多
Exploitation of oxygen evolution reaction(OER)and urea oxidation reaction(UOR)catalysts with high activity and stability at large current density is a major challenge for energy-saving H_(2) production in water electr...Exploitation of oxygen evolution reaction(OER)and urea oxidation reaction(UOR)catalysts with high activity and stability at large current density is a major challenge for energy-saving H_(2) production in water electrolysis.Herein,we use the pyridinic-N doping carbon layers coupled with tensile strain of FeNi alloy activated by NiFe_(2)O_(4)(FeNi/NiFe_(2)O_(4)@NC)for efficiently increasing the performance of water and urea oxidation.Due to the tensile strain effect on FeNi/NiFe_(2)O_(4)@NC,it provides a favorable modulation on the electronic properties of the active center,thus enabling amazing OER(η_(100)=196 mV)and UOR(E_(10)=1.32 V)intrinsic activity.Besides,the carbon-coated layers can be used as armor to prevent FeNi alloy from being corroded by the electrolyte for enhancing the OER/UOR stability at large current density,showing high industrial practicability.This work thus provides a simple way to prepare high-efficiency catalyst for activating water and urea oxidation.展开更多
Urea oxidation reaction(UOR) has been selected as substitution for oxygen evolution reaction ascribing to its low thermodynamic voltage as well as utilization of nickel as electrocatalyst.Herein,we report the formatio...Urea oxidation reaction(UOR) has been selected as substitution for oxygen evolution reaction ascribing to its low thermodynamic voltage as well as utilization of nickel as electrocatalyst.Herein,we report the formation of nickel single atoms(Ni-SAs) as exceptional bifunctional electrocatalyst toward UOR and hydrogen evolution reaction(HER) in urea-assisted water splitting.In UOR catalysis,Ni-SAs perform a superior catalytic performance than Ni-NP/NC and Pt/C ascribing to the formation of HOO-Ni-N_(4) structure evidenced by in-situ Raman spectroscopy,corresponding to a boosted mass activity by 175-fold at 1.4 V vs.RHE than Ni-NP/NC.Furthermore,Ni-SAs requires only 450 mV overpotential to obtain HER current density of 500 mA cm^(-2).136 mA cm^(-2) is achieved in urea-assisted water splitting at1.7 V for Ni-SAs,boosted by 5.7 times than Pt/C-IrO_(2) driven water splitting.展开更多
Interfacial electronic structure modulation of nickel-based electrocata-lysts is significant in boosting energy-conversion-relevant urea oxidation reaction(UOR).Herein,porous carbon nanofibers confined mixed Ni-based ...Interfacial electronic structure modulation of nickel-based electrocata-lysts is significant in boosting energy-conversion-relevant urea oxidation reaction(UOR).Herein,porous carbon nanofibers confined mixed Ni-based crystal phases of Ni_(2)P and NiF_(2) are developed via fluorination and phosphorization of Ni coated carbon nanofiber(Ni_(2)P/NiF_(2)/PCNF),which possess sufficient mesoporous and optimized Gibbs adsorption free energy by mixed phase-induced charge redistribution.This novel system further reduces the reaction energy barrier and improves the reaction activity by addressing the challenges of low intrinsic activity,difficulty in active site formation,and insufficient synergism.A considerably high current density of 254.29 mA cm^(-2) is reached at 1.54 V versus reversible hydrogen electrode on a glass carbon electrode,and the cell voltage requires 1.39 V to get 10 mA cm^(-2) in hydrogen generation,with very good stability,about 190 mV less than that of the traditional water electrolysis.The facile active phase formation and high charge transfer ability induced by asymmetric charge redistribution are found in the interface,where the urea molecules tend to bond with Ni atoms on the surface of heterojunction,and the rate-determining step is changed from CO_(2) desorption to the fourth H-atom deprotonation.The work reveals a novel catalyst system by interfacial charge redistribution induced by high bond polarity for energy-relevant catalysis reactions.展开更多
Urea-assisted natural seawater electrolysis is an emerging technology that is effective for grid-scale carbon-neutral hydrogen mass production yet challenging.Circumventing scaling relations is an effective strategy t...Urea-assisted natural seawater electrolysis is an emerging technology that is effective for grid-scale carbon-neutral hydrogen mass production yet challenging.Circumventing scaling relations is an effective strategy to break through the bottleneck of natural seawater splitting.Herein,by DFT calculation,we demonstrated that the interface boundaries between Ni_(2)P and MoO_(2) play an essential role in the selfrelaxation of the Ni-O interfacial bond,effectively modulating a coordination number of intermediates to control independently their adsorption-free energy,thus circumventing the adsorption-energy scaling relation.Following this conceptual model,a well-defined 3D F-doped Ni_(2)P-MoO_(2) heterostructure microrod array was rationally designed via an interfacial engineering strategy toward urea-assisted natural seawater electrolysis.As a result,the F-Ni_(2)P-MoO_(2) exhibits eminently active and durable bifunctional catalysts for both HER and OER in acid,alkaline,and alkaline sea water-based electrolytes.By in-situ analysis,we found that a thin amorphous layer of NiOOH,which is evolved from the Ni_(2)P during anodic reaction,is real catalytic active sites for the OER and UOR processes.Remarkable,such electrode-assembled urea-assisted natural seawater electrolyzer requires low voltages of 1.29 and 1.75 V to drive 10 and600 mA cm^(-2)and demonstrates superior durability by operating continuously for 100 h at 100 mA cm^(-2),beyond commercial Pt/C||RuO_(2) and most previous reports.展开更多
Urea and oxalic acid are critical component in various chemical manufacturing industries.However,achieving simultaneous generation of urea and oxalic acid in a continuous-flow electrolyzer is a challenge.Herein,we rep...Urea and oxalic acid are critical component in various chemical manufacturing industries.However,achieving simultaneous generation of urea and oxalic acid in a continuous-flow electrolyzer is a challenge.Herein,we report a continuous-flow electrolyzer equipped with 9-square centime-ter-effective area gas diffusion electrodes(GDE)which can simultaneously catalyze the glycerol oxidation reaction in the anode region and the reduction reaction of CO_(2) and nitrate in the cathode region,producing oxalic acid and urea at both the anode and cathode,respectively.The current density at low cell voltage(0.9 V)remained above 18.7 mA cm^(-2) for 10 consecutive electrolysis cycles(120 h in total),and the Faraday efficiency of oxalic acid(67.1%) and urea(70.9%)did not decay.Experimental and theoretical studies show that in terms of the formation of C-N bond at the cathode,Pd-sites can provide protons for the hydrogenation process of CO_(2) and NO_(3)^(-),Cu-sites can promote the generation of *COOH and Bi-sites can stabilize *COOH.In addition,in terms of glycerol oxidation,the introduction of Cu and Bi into Pd metallene promotes the oxidation of hydroxyl groups and the cleavage of C-C bond in glycerol molecules,respectively.展开更多
Electrocatalytic urea synthesis provides a favorable strategy for conventional energy-consuming urea synthesis,but achieving large-scale catalyst synthesis with high catalytic efficiency remains challenging.Herein,we ...Electrocatalytic urea synthesis provides a favorable strategy for conventional energy-consuming urea synthesis,but achieving large-scale catalyst synthesis with high catalytic efficiency remains challenging.Herein,we developed a simple method for the preparation of a series of FeNi-alloy-based catalysts,named FeNi@nC-T(n represents the content of nanoporous carbon as 1,3,5,7 or 9 g and T=900,950,1000 or 1100°C),for highly performed urea synthesis via NO_(3)−and CO_(2)co-reduction.The FeNi@7C-1000 achieved a high urea yield of 1041.33 mmol h^(−1)gFeNi^(−1)with a Faradaic efficiency of 15.56%at–1.2 V vs.RHE.Moreover,the scale-up synthesized FeNi@7C-950-S(over 140 g per batch)was achieved with its high catalytic performance and high stability maintained.Mechanism investigation illuminated that the Ni and Fe sites catalyze and stabilize the key*CO and*N intermediates and minimize the C–N coupling reaction barriers for highly efficient urea synthesis.展开更多
Controlled-release urea(CRU)is commonly used to improve the crop yield and nitrogen use efficiency(NUE).However,few studies have investigated the effects of CRU in the ratoon rice system.Ratoon rice is the practice of...Controlled-release urea(CRU)is commonly used to improve the crop yield and nitrogen use efficiency(NUE).However,few studies have investigated the effects of CRU in the ratoon rice system.Ratoon rice is the practice of obtaining a second harvest from tillers originating from the stubble of the previously harvested main crop.In this study,a 2-year field experiment using a randomized complete block design was conducted to determine the effects of CRU on the yield,NUE,and economic benefits of ratoon rice,including the main crop,to provide a theoretical basis for fertilization of ratoon rice.The experiment included four treatments:(i)no N fertilizer(CK);(ii)traditional practice with 5 applications of urea applied at different crop growth stages by surface broadcasting(FFP);(iii)one-time basal application of CRU(BF1);and(iv)one-time basal application of CRU combined with common urea(BF2).The BF1 and BF2 treatments significantly increased the main crop yield by 17.47 and 15.99%in 2019,and by 17.91 and 16.44%in 2020,respectively,compared with FFP treatment.The BF2 treatment achieved similar yield of the ratoon crop to the FFP treatment,whereas the BF1 treatment significantly increased the yield of the ratoon crop by 14.81%in 2019 and 12.21%in 2020 compared with the FFP treatment.The BF1 and BF2 treatments significantly improved the 2-year apparent N recovery efficiency,agronomic NUE,and partial factor productivity of applied N by 11.47-16.66,27.31-44.49,and 9.23-15.60%,respectively,compared with FFP treatment.The BF1 and BF2 treatments reduced the chalky rice rate and chalkiness of main and ratoon crops relative to the FFP treatment.Furthermore,emergy analysis showed that the production efficiency of the BF treatments was higher than that of the FFP treatment.The BF treatments reduced labor input due to reduced fertilization times and improved the economic benefits of ratoon rice.Compared with the FFP treatment,the BF1 and BF2 treatments increased the net income by 14.21-16.87 and 23.76-25.96%,respectively.Overall,the one-time blending use of CRU and common urea should be encouraged to achieve high yield,high nitrogen use efficiency,and good quality of ratoon rice,which has low labor input and low apparent N loss.展开更多
Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)...Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen electrode.Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~*NHO.This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.展开更多
Electrochemical co-reduction of nitrate(NO_(3)^(-))and carbon dioxide(CO_(2))has been widely regarded as a promising route to produce urea under ambient conditions,however the yield rate of urea has remained limited.H...Electrochemical co-reduction of nitrate(NO_(3)^(-))and carbon dioxide(CO_(2))has been widely regarded as a promising route to produce urea under ambient conditions,however the yield rate of urea has remained limited.Here,we report an atomically ordered intermetallic pallium-zinc(PdZn)electrocatalyst comprising a high density of PdZn pairs for boosting urea electrosynthesis.It is found that Pd and Zn are responsible for the adsorption and activation of NO_(3)^(-)and CO_(2),respectively,and thus the co-adsorption and co-activation NO_(3)^(-)and CO_(2) are achieved in ordered PdZn pairs.More importantly,the ordered and well-defined PdZn pairs provide a dual-site geometric structure conducive to the key C-N coupling with a low kinetical barrier,as demonstrated on both operando measurements and theoretical calculations.Consequently,the PdZn electrocatalyst displays excellent performance for the co-reduction to generate urea with a maximum urea Faradaic efficiency of 62.78%and a urea yield rate of 1274.42μg mg^(-1) h^(-1),and the latter is 1.5-fold larger than disordered pairs in PdZn alloys.This work paves new pathways to boost urea electrosynthesis via constructing ordered dual-metal pairs.展开更多
BACKGROUND Helicobacter pylori(H.pylori)infection has been well-established as a significant risk factor for several gastrointestinal disorders.The urea breath test(UBT)has emerged as a leading non-invasive method for...BACKGROUND Helicobacter pylori(H.pylori)infection has been well-established as a significant risk factor for several gastrointestinal disorders.The urea breath test(UBT)has emerged as a leading non-invasive method for detecting H.pylori.Despite numerous studies confirming its substantial accuracy,the reliability of UBT results is often compromised by inherent limitations.These findings underscore the need for a rigorous statistical synthesis to clarify and reconcile the diagnostic accuracy of the UBT for the diagnosis of H.pylori infection.AIM To determine and compare the diagnostic accuracy of 13C-UBT and 14C-UBT for H.pylori infection in adult patients with dyspepsia.METHODS We conducted an independent search of the PubMed/MEDLINE,EMBASE,and Cochrane Central databases until April 2022.Our search included diagnostic accuracy studies that evaluated at least one of the index tests(^(13)C-UBT or ^(14)C-UBT)against a reference standard.We used the QUADAS-2 tool to assess the methodo-logical quality of the studies.We utilized the bivariate random-effects model to calculate sensitivity,specificity,positive and negative test likelihood ratios(LR+and LR-),as well as the diagnostic odds ratio(DOR),and their 95%confidence intervals.We conducted subgroup analyses based on urea dosing,time after urea administration,and assessment technique.To investigate a possible threshold effect,we conducted Spearman correlation analysis,and we generated summary receiver operating characteristic(SROC)curves to assess heterogeneity.Finally,we visually inspected a funnel plot and used Egger’s test to evaluate publication bias.endorsing both as reliable diagnostic tools in clinical practice.CONCLUSION In summary,our study has demonstrated that ^(13)C-UBT has been found to outperform the ^(14)C-UBT,making it the preferred diagnostic approach.Additionally,our results emphasize the significance of carefully considering urea dosage,assessment timing,and measurement techniques for both tests to enhance diagnostic precision.Nevertheless,it is crucial for researchers and clinicians to evaluate the strengths and limitations of our findings before implementing them in practice.展开更多
Urea oxidation reaction(UOR)is proposed as an exemplary half-reaction in renewable energy applications because of its low thermodynamical potential.However,challenges persist due to sluggish reaction kinetics and comp...Urea oxidation reaction(UOR)is proposed as an exemplary half-reaction in renewable energy applications because of its low thermodynamical potential.However,challenges persist due to sluggish reaction kinetics and complex by-products separation.To this end,we introduce the lattice oxygen oxidation mechanism(LOM),propelling a novel UOR route using a modified CoFe layered double hydroxide(LDH)catalyst termed CFRO-7.Theoretical calculations and in-situ characterizations highlight the activated lattice oxygen(O_(L))within CFRO-7 as pivotal sites for UOR,optimizing the reaction pathway and accelerating the kinetics.For the urea overall electrolysis application,the LOM route only requires a low voltage of 1.54 V to offer a high current of 100 mA cm^(-2) for long-term utilization(>48 h).Importantly,the by-product NCO^(-)−is significantly suppressed,while the CO_(2)2/N_(2) separation is efficiently achieved.This work proposed a pioneering paradigm,invoking the LOM pathway in urea electrolysis to expedite reaction dynamics and enhance product selectivity.展开更多
In this editorial,we discuss the article in the World Journal of Gastroenterology.The article conducts a meta-analysis of the diagnostic accuracy of the urea breath test(UBT),a non-invasive method for detecting Helico...In this editorial,we discuss the article in the World Journal of Gastroenterology.The article conducts a meta-analysis of the diagnostic accuracy of the urea breath test(UBT),a non-invasive method for detecting Helicobacter pylori(H.pylori)infection in humans.It is based on radionuclide-labeled urea.Various methods,both invasive and non-invasive,are available for diagnosing H.pylori infection,inclu-ding endoscopy with biopsy,serology for immunoglobulin titers,stool antigen analysis,and UBT.Several guidelines recommend UBTs as the primary choice for diagnosing H.pylori infection and for reexamining after eradication therapy.It is used to be the first choice non-invasive test due to their high accuracy,specificity,rapid results,and simplicity.Moreover,its performance remains unaffected by the distribution of H.pylori in the stomach,allowing a high flow of patients to be tested.Despite its widespread use,the performance characteristics of UBT have been inconsistently described and remain incompletely defined.There are two UBTs available with Food and Drug Administration approval:The 13C and 14C tests.Both tests are affordable and can provide real-time results.Physicians may prefer the 13C test because it is non-radioactive,compared to 14C which uses a radioactive isotope,especially in young children and pregnant women.Although there was heterogeneity among the studies regarding the diagnostic accuracy of both UBTs,13C-UBT consistently outperforms the 14C-UBT.This makes the 13C-UBT the preferred diagnostic approach.Furthermore,the provided findings of the meta-analysis emphasize the significance of precise considerations when choosing urea dosage,assessment timing,and measurement techniques for both the 13C-UBT and 14C-UBT,to enhance diagnostic precision.展开更多
Controllable design of the catalytic electrodes with hierarchical superstructures is expected to improve their electrochemical performance.Herein,a self-supported integrated electrode(NiCo-ZLDH/NF)with a unique hierar...Controllable design of the catalytic electrodes with hierarchical superstructures is expected to improve their electrochemical performance.Herein,a self-supported integrated electrode(NiCo-ZLDH/NF)with a unique hierarchical quaternary superstructure was fabricated through a self-sacrificing template strategy from the metal–organic framework(Co-ZIF-67)nanoplate arrays,which features an intriguing well-defined hierarchy when taking the unit cells of the NiCo-based layered double hydroxide(NiCo-LDH)as the primary structure,the ultrathin LDH nanoneedles as the secondary structure,the mesoscale hollow plates of the LDH nanoneedle arrays as the tertiary structure,and the macroscale three-dimensional frames of the plate arrays as the quaternary structure.Notably,the distinctive structure of NiCo-ZLDH/NF can not only accelerate both mass and charge transfer,but also expose plentiful accessible active sites with high intrinsic activity,endowing it with an excellent electrochemical performance for urea oxidation reaction(UOR).Specially,it only required the low potentials of 1.335,1.368 and 1.388 V to deliver the current densities of 10,100 and 200 mA cm^(-2),respectively,much superior to those for typical NiCo-LDH.Employing NiCo-ZLDH/NF as the bifunctional electrode for both anodic UOR and cathodic HER,an energy-saving electrolysis system was further explored which can greatly reduce the needed voltage of 213 mV to deliver the current density of 100 mA cm^(-2),as compared to the conventional water electrolysis system composed of OER.This work manifests that it is prospective to explore the hierarchically nanostructured electrodes and the innovative electrolytic technologies for high-efficiency electrocatalysis.展开更多
Urea synthesis through the simultaneous electrocatalytic reduction of N_(2)and CO_(2)molecules under ambient conditions holds great promises as a sustainable alternative to its industrial production,in which the devel...Urea synthesis through the simultaneous electrocatalytic reduction of N_(2)and CO_(2)molecules under ambient conditions holds great promises as a sustainable alternative to its industrial production,in which the development of stable,highly efficient,and highly selective catalysts to boost the chemisorption,activation,and coupling of inert N_(2)and CO_(2)molecules remains rather challenging.Herein,by means of density functional theory computations,we proposed a new class of two-dimensional nanomaterials,namely,transition-metal phosphide monolayers(TM_(2)P,TM=Ti,Fe,Zr,Mo,and W),as the potential electrocatalysts for urea production.Our results showed that these TM_(2)P materials exhibit outstanding stability and excellent metallic properties.Interestingly,the Mo_(2)P monolayer was screened out as the best catalyst for urea synthesis due to its small kinetic energy barrier(0.35 eV)for C-N coupling,low limiting potential(-0.39 V),and significant suppressing effects on the competing side reactions.The outstanding catalytic activity of the Mo_(2)P monolayer can be ascribed to its optimal adsorption strength with the key^(*)NCON species due to its moderate positive charges on the Mo active sites.Our findings not only propose a novel catalyst with high-efficiency and high-selectivity for urea production but also further widen the potential applications of metal phosphides in electrocatalysis.展开更多
Urea is widely used as fertilizer and is a key substance supporting global food production. However, the traditional industrial synthesis of urea faces the challenges with high energy consumption and serious environme...Urea is widely used as fertilizer and is a key substance supporting global food production. However, the traditional industrial synthesis of urea faces the challenges with high energy consumption and serious environmental problems. With the increasing global demand for environmental protection and sustainable development, it is much necessary to develop novel and clean methods for the synthesis of urea.Electrocatalysis provides an efficient and renewable synthesis route that can directly produce urea at room temperature and atmospheric pressure by the coupling of CO_(2) and nitrogenous molecules. In this review, we summarized the most recent advances in electrochemical synthesis of urea via CAN coupling systematically, focusing on the coupling of CO_(2) and different nitrogen sources. And the associated coupling mechanism, catalysts optimization, and electrolyzer design are well discussed. Moreover, the challenges and future directions for electrocatalytic CAN coupling are prospected. This review will provide timely and valuable guidance for others and attract more interests to promote the development of electrochemical synthesis of urea or other valuable chemicals containing CAN bond.展开更多
The combined effects of straw incorporation(SI)and polymer-coated urea(PCU)application on soil ammonia(NH_(3))and nitrous oxide(N_(2)O)emissions from agricultural fields have not been comprehensively evaluated in Nort...The combined effects of straw incorporation(SI)and polymer-coated urea(PCU)application on soil ammonia(NH_(3))and nitrous oxide(N_(2)O)emissions from agricultural fields have not been comprehensively evaluated in Northwest China.We conducted a two-year field experiment to assess the effects of combining SI with either uncoated urea(U)or PCU on soil NH_(3)emissions,N_(2)O emissions,winter wheat yields,yield-scaled NH_(3)(/NH_(3)),and yield-scaled N_(2)O(/N_(2)O).Five treatments were investigated,no nitrogen(N)fertilizer(N_(0)),U application at 150 kg N ha-1 with and without SI(SI+U and S_(0)+U),and PCU application at 150 kg N ha^(-1) with and without SI(SI+PCU and S_(0)+PCU).The results showed that the NH_(3);emissions increased by 20.98-34.35%following Sl compared to straw removal,mainly due to increases in soil ammonium(NH_(4)^(+)-N)content and water-flled pore space(WFPS).SI resulted in higher N_(2)O emissions than under the So scenario by 13.31-49.23%due to increases in soil inorganic N(SIN)contents,WFPS,and soil microbial biomass.In contrast,the PCU application reduced the SIN contents compared to the U application,reducing the NH_(3)and N_(2)O emissions by 45.99-58.07 and 18.08-53.04%,respectively.Moreover,no significant positive effects of the SI or PCU applications on the winter wheat yield were observed.The lowest /NH_(3) and /N_(2)O values were observed under the S_(0)+PCU and SI+PCU treatments.Our results suggest that single PCU applications and their combination with straw are the optimal agricultural strategies for mitigating gaseous N emissions and maintaining optimal winter wheat yields in Northwest China.展开更多
Metabolic reprogramming is a key feature driving oncogenesis in cancers. Recent studies have revealed that protein metabolism is largely altered in gliomas facilitating its malignant growth. Urea is the end product of...Metabolic reprogramming is a key feature driving oncogenesis in cancers. Recent studies have revealed that protein metabolism is largely altered in gliomas facilitating its malignant growth. Urea is the end product of nitrogen metabolism which is mainly produced by arginase. The interdependence of arginase and other biochemical mechanisms triggered scientific research interest. This research aimed to investigate the relationships between the urea as the main parameter of protein metabolism and glioma progression. It was also the most pronounced relationship between urea and the level of the nuclear protein Ki-67 as a marker of proliferative activity and O-6-methylguanine-DNA methyltransferase (MGMT), which performs DNA repair. Postoperative material from 20 patients with gliomas of different grades of anaplasia was analyzed.展开更多
基金financial support from the National Natural Science Foundation of China(52203070)the Open Fund of State Key Laboratory of New Textile Materials and Advanced Processing Technologies(FZ2022005)+2 种基金the Open Fund of Hubei Key Laboratory of Biomass Fiber and Ecological Dyeing and Finishing(STRZ202203)the financial support provided by the China Scholarship Council(CSC)Visiting Scholar Programfinancial support from Institute for Sustainability,Energy and Resources,The University of Adelaide,Future Making Fellowship。
文摘Urea holds promise as an alternative water-oxidation substrate in electrolytic cells.High-valence nickelbased spinel,especially after heteroatom doping,excels in urea oxidation reactions(UOR).However,traditional spinel synthesis methods with prolonged high-temperature reactions lack kinetic precision,hindering the balance between controlled doping and highly active two-dimensional(2D)porous structures design.This significantly impedes the identification of electron configuration-dependent active sites in doped 2D nickel-based spinels.Herein,we present a microwave shock method for the preparation of 2D porous NiCo_(2)O_(4)spinel.Utilizing the transient on-off property of microwave pulses for precise heteroatom doping and 2D porous structural design,non-metal doping(boron,phosphorus,and sulfur)with distinct extranuclear electron disparities serves as straightforward examples for investigation.Precise tuning of lattice parameter reveals the impact of covalent bond strength on NiCo_(2)O_(4)structural stability.The introduced defect levels induce unpaired d-electrons in transition metals,enhancing the adsorption of electron-donating amino groups in urea molecules.Simultaneously,Bode plots confirm the impact mechanism of rapid electron migration caused by reduced band gaps on UOR activity.The prepared phosphorus-doped 2D porous NiCo_(2)O_(4),with optimal electron configuration control,outperforms most reported spinels.This controlled modification strategy advances understanding theoretical structure-activity mechanisms of high-performance 2D spinels in UOR.
基金financially supported by the National Key R&D Program of China(2022YFA1503003)the National Natural Science Foundation of China(91961111,22271081)+3 种基金the Natural Science Foundation of Heilongjiang Province(ZD2021B003)the University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(UNPYSCT-2020004)The Basic Research Fund of Heilongjiang University in Heilongjiang Province(2021-KYYWF-0039)the Heilongjiang University Excellent Youth Foundation。
文摘Hydrogen evolution reaction(HER)and urea oxidation reaction(UOR)are key reactions of the watercycling associated catalytic process/device.The design of catalysts with a super-hydrophilic/aerophobic structure and optimized electron distribution holds great promise.Here,we have designed a threedimensional(3D)hollow Ni/NiMoN hierarchical structure with arrayed-sheet surface based on a onepot hydrothermal route for efficient urea-assisted HER based on a simple hydrothermal process.The Ni/NiMoN catalyst exhibits super-hydrophilic/aerophobic properties with a small droplet contact angle of 6.07°and an underwater bubble contact angle of 155.7°,thus facilitating an escape of bubbles from the electrodes.Density functional theory calculations and X-ray photoelectron spectroscopy results indicate the optimized electronic structure at the interface of Ni and NiMoN,which can promote the adsorption/desorption of reactants and intermediates.The virtues combining with a large specific surface area endow Ni/NiMoN with efficient catalytic activity of low potentials of 25 mV for HER and 1.33 V for UOR at10 mA cm^(-2).The coupled HER and UOR system demonstrates a low cell voltage of 1.42 V at 10 mA cm^(-2),which is approximately 209 mV lower than water electrolysis.
基金supported by the National Natural Science Foundation of China(21872040,22162004)the Excellent Scholars and Innovation Team of Guangxi Universities,the Innovation Project of Guangxi Graduate Education(YCBZ2022038)the High-performance Computing Platform of Guangxi University.
文摘Exploitation of oxygen evolution reaction(OER)and urea oxidation reaction(UOR)catalysts with high activity and stability at large current density is a major challenge for energy-saving H_(2) production in water electrolysis.Herein,we use the pyridinic-N doping carbon layers coupled with tensile strain of FeNi alloy activated by NiFe_(2)O_(4)(FeNi/NiFe_(2)O_(4)@NC)for efficiently increasing the performance of water and urea oxidation.Due to the tensile strain effect on FeNi/NiFe_(2)O_(4)@NC,it provides a favorable modulation on the electronic properties of the active center,thus enabling amazing OER(η_(100)=196 mV)and UOR(E_(10)=1.32 V)intrinsic activity.Besides,the carbon-coated layers can be used as armor to prevent FeNi alloy from being corroded by the electrolyte for enhancing the OER/UOR stability at large current density,showing high industrial practicability.This work thus provides a simple way to prepare high-efficiency catalyst for activating water and urea oxidation.
基金supported by the National Natural Science Foundation of China(No.22209126)。
文摘Urea oxidation reaction(UOR) has been selected as substitution for oxygen evolution reaction ascribing to its low thermodynamic voltage as well as utilization of nickel as electrocatalyst.Herein,we report the formation of nickel single atoms(Ni-SAs) as exceptional bifunctional electrocatalyst toward UOR and hydrogen evolution reaction(HER) in urea-assisted water splitting.In UOR catalysis,Ni-SAs perform a superior catalytic performance than Ni-NP/NC and Pt/C ascribing to the formation of HOO-Ni-N_(4) structure evidenced by in-situ Raman spectroscopy,corresponding to a boosted mass activity by 175-fold at 1.4 V vs.RHE than Ni-NP/NC.Furthermore,Ni-SAs requires only 450 mV overpotential to obtain HER current density of 500 mA cm^(-2).136 mA cm^(-2) is achieved in urea-assisted water splitting at1.7 V for Ni-SAs,boosted by 5.7 times than Pt/C-IrO_(2) driven water splitting.
基金The work was supported by the National Natural Science Foundation of China(22272148,21972124)Chun Yin thanks the support of Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX24_3720).
文摘Interfacial electronic structure modulation of nickel-based electrocata-lysts is significant in boosting energy-conversion-relevant urea oxidation reaction(UOR).Herein,porous carbon nanofibers confined mixed Ni-based crystal phases of Ni_(2)P and NiF_(2) are developed via fluorination and phosphorization of Ni coated carbon nanofiber(Ni_(2)P/NiF_(2)/PCNF),which possess sufficient mesoporous and optimized Gibbs adsorption free energy by mixed phase-induced charge redistribution.This novel system further reduces the reaction energy barrier and improves the reaction activity by addressing the challenges of low intrinsic activity,difficulty in active site formation,and insufficient synergism.A considerably high current density of 254.29 mA cm^(-2) is reached at 1.54 V versus reversible hydrogen electrode on a glass carbon electrode,and the cell voltage requires 1.39 V to get 10 mA cm^(-2) in hydrogen generation,with very good stability,about 190 mV less than that of the traditional water electrolysis.The facile active phase formation and high charge transfer ability induced by asymmetric charge redistribution are found in the interface,where the urea molecules tend to bond with Ni atoms on the surface of heterojunction,and the rate-determining step is changed from CO_(2) desorption to the fourth H-atom deprotonation.The work reveals a novel catalyst system by interfacial charge redistribution induced by high bond polarity for energy-relevant catalysis reactions.
基金supported by the Vietnam National University,Ho Chi Minh City (Grant No.TX2024-50-01)partial supported by National Natural Science Foundation of China (Grant No.22209186)。
文摘Urea-assisted natural seawater electrolysis is an emerging technology that is effective for grid-scale carbon-neutral hydrogen mass production yet challenging.Circumventing scaling relations is an effective strategy to break through the bottleneck of natural seawater splitting.Herein,by DFT calculation,we demonstrated that the interface boundaries between Ni_(2)P and MoO_(2) play an essential role in the selfrelaxation of the Ni-O interfacial bond,effectively modulating a coordination number of intermediates to control independently their adsorption-free energy,thus circumventing the adsorption-energy scaling relation.Following this conceptual model,a well-defined 3D F-doped Ni_(2)P-MoO_(2) heterostructure microrod array was rationally designed via an interfacial engineering strategy toward urea-assisted natural seawater electrolysis.As a result,the F-Ni_(2)P-MoO_(2) exhibits eminently active and durable bifunctional catalysts for both HER and OER in acid,alkaline,and alkaline sea water-based electrolytes.By in-situ analysis,we found that a thin amorphous layer of NiOOH,which is evolved from the Ni_(2)P during anodic reaction,is real catalytic active sites for the OER and UOR processes.Remarkable,such electrode-assembled urea-assisted natural seawater electrolyzer requires low voltages of 1.29 and 1.75 V to drive 10 and600 mA cm^(-2)and demonstrates superior durability by operating continuously for 100 h at 100 mA cm^(-2),beyond commercial Pt/C||RuO_(2) and most previous reports.
文摘Urea and oxalic acid are critical component in various chemical manufacturing industries.However,achieving simultaneous generation of urea and oxalic acid in a continuous-flow electrolyzer is a challenge.Herein,we report a continuous-flow electrolyzer equipped with 9-square centime-ter-effective area gas diffusion electrodes(GDE)which can simultaneously catalyze the glycerol oxidation reaction in the anode region and the reduction reaction of CO_(2) and nitrate in the cathode region,producing oxalic acid and urea at both the anode and cathode,respectively.The current density at low cell voltage(0.9 V)remained above 18.7 mA cm^(-2) for 10 consecutive electrolysis cycles(120 h in total),and the Faraday efficiency of oxalic acid(67.1%) and urea(70.9%)did not decay.Experimental and theoretical studies show that in terms of the formation of C-N bond at the cathode,Pd-sites can provide protons for the hydrogenation process of CO_(2) and NO_(3)^(-),Cu-sites can promote the generation of *COOH and Bi-sites can stabilize *COOH.In addition,in terms of glycerol oxidation,the introduction of Cu and Bi into Pd metallene promotes the oxidation of hydroxyl groups and the cleavage of C-C bond in glycerol molecules,respectively.
文摘Electrocatalytic urea synthesis provides a favorable strategy for conventional energy-consuming urea synthesis,but achieving large-scale catalyst synthesis with high catalytic efficiency remains challenging.Herein,we developed a simple method for the preparation of a series of FeNi-alloy-based catalysts,named FeNi@nC-T(n represents the content of nanoporous carbon as 1,3,5,7 or 9 g and T=900,950,1000 or 1100°C),for highly performed urea synthesis via NO_(3)−and CO_(2)co-reduction.The FeNi@7C-1000 achieved a high urea yield of 1041.33 mmol h^(−1)gFeNi^(−1)with a Faradaic efficiency of 15.56%at–1.2 V vs.RHE.Moreover,the scale-up synthesized FeNi@7C-950-S(over 140 g per batch)was achieved with its high catalytic performance and high stability maintained.Mechanism investigation illuminated that the Ni and Fe sites catalyze and stabilize the key*CO and*N intermediates and minimize the C–N coupling reaction barriers for highly efficient urea synthesis.
基金supported by the Key R&D Plan of Hubei Province,China(2022BBA002)the Carbon Account Accounting and Carbon Reduction and Sequestration Technology Research of Quzhou City of China(2022-31).
文摘Controlled-release urea(CRU)is commonly used to improve the crop yield and nitrogen use efficiency(NUE).However,few studies have investigated the effects of CRU in the ratoon rice system.Ratoon rice is the practice of obtaining a second harvest from tillers originating from the stubble of the previously harvested main crop.In this study,a 2-year field experiment using a randomized complete block design was conducted to determine the effects of CRU on the yield,NUE,and economic benefits of ratoon rice,including the main crop,to provide a theoretical basis for fertilization of ratoon rice.The experiment included four treatments:(i)no N fertilizer(CK);(ii)traditional practice with 5 applications of urea applied at different crop growth stages by surface broadcasting(FFP);(iii)one-time basal application of CRU(BF1);and(iv)one-time basal application of CRU combined with common urea(BF2).The BF1 and BF2 treatments significantly increased the main crop yield by 17.47 and 15.99%in 2019,and by 17.91 and 16.44%in 2020,respectively,compared with FFP treatment.The BF2 treatment achieved similar yield of the ratoon crop to the FFP treatment,whereas the BF1 treatment significantly increased the yield of the ratoon crop by 14.81%in 2019 and 12.21%in 2020 compared with the FFP treatment.The BF1 and BF2 treatments significantly improved the 2-year apparent N recovery efficiency,agronomic NUE,and partial factor productivity of applied N by 11.47-16.66,27.31-44.49,and 9.23-15.60%,respectively,compared with FFP treatment.The BF1 and BF2 treatments reduced the chalky rice rate and chalkiness of main and ratoon crops relative to the FFP treatment.Furthermore,emergy analysis showed that the production efficiency of the BF treatments was higher than that of the FFP treatment.The BF treatments reduced labor input due to reduced fertilization times and improved the economic benefits of ratoon rice.Compared with the FFP treatment,the BF1 and BF2 treatments increased the net income by 14.21-16.87 and 23.76-25.96%,respectively.Overall,the one-time blending use of CRU and common urea should be encouraged to achieve high yield,high nitrogen use efficiency,and good quality of ratoon rice,which has low labor input and low apparent N loss.
基金supported by the Research Grants Council(26206115,16304821 and 16309418)the Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou)(SMSEGL20SC01)+2 种基金the Innovation and Technology Commission(grant no.ITC-CNERC14EG03)of the Hong Kong Special Administrative Regionthe Hong Kong Postdoctoral Fellowship Scheme(HKUST PDFS2021-4S12 and HKUST PDFS2021-6S08)the support from the Shenzhen fundamental research funding(JCYJ20210324115809026,20200925154115001,JCYJ20200109141216566)。
文摘Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen electrode.Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~*NHO.This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.
基金supported by the National Natural Science Foundation of China(22379100,U21A20312)the Shenzhen Science and Technology Program(Grant No.20231121200418001)+1 种基金the Guangdong Basic and Applied Basic Research Foundation(2022B1515120084)the Key Project of Department of Education of Guangdong Province(2023ZDZX3020)。
文摘Electrochemical co-reduction of nitrate(NO_(3)^(-))and carbon dioxide(CO_(2))has been widely regarded as a promising route to produce urea under ambient conditions,however the yield rate of urea has remained limited.Here,we report an atomically ordered intermetallic pallium-zinc(PdZn)electrocatalyst comprising a high density of PdZn pairs for boosting urea electrosynthesis.It is found that Pd and Zn are responsible for the adsorption and activation of NO_(3)^(-)and CO_(2),respectively,and thus the co-adsorption and co-activation NO_(3)^(-)and CO_(2) are achieved in ordered PdZn pairs.More importantly,the ordered and well-defined PdZn pairs provide a dual-site geometric structure conducive to the key C-N coupling with a low kinetical barrier,as demonstrated on both operando measurements and theoretical calculations.Consequently,the PdZn electrocatalyst displays excellent performance for the co-reduction to generate urea with a maximum urea Faradaic efficiency of 62.78%and a urea yield rate of 1274.42μg mg^(-1) h^(-1),and the latter is 1.5-fold larger than disordered pairs in PdZn alloys.This work paves new pathways to boost urea electrosynthesis via constructing ordered dual-metal pairs.
基金Supported by Scientific Initiation Scholarship Programme(PIBIC)of the Bahia State Research Support Foundationthe Doctorate Scholarship Program of the Coordination of Improvement of Higher Education Personnel+1 种基金the Scientific Initiation Scholarship Programme(PIBIC)of the National Council for Scientific and Technological Developmentand the CNPq Research Productivity Fellowship.
文摘BACKGROUND Helicobacter pylori(H.pylori)infection has been well-established as a significant risk factor for several gastrointestinal disorders.The urea breath test(UBT)has emerged as a leading non-invasive method for detecting H.pylori.Despite numerous studies confirming its substantial accuracy,the reliability of UBT results is often compromised by inherent limitations.These findings underscore the need for a rigorous statistical synthesis to clarify and reconcile the diagnostic accuracy of the UBT for the diagnosis of H.pylori infection.AIM To determine and compare the diagnostic accuracy of 13C-UBT and 14C-UBT for H.pylori infection in adult patients with dyspepsia.METHODS We conducted an independent search of the PubMed/MEDLINE,EMBASE,and Cochrane Central databases until April 2022.Our search included diagnostic accuracy studies that evaluated at least one of the index tests(^(13)C-UBT or ^(14)C-UBT)against a reference standard.We used the QUADAS-2 tool to assess the methodo-logical quality of the studies.We utilized the bivariate random-effects model to calculate sensitivity,specificity,positive and negative test likelihood ratios(LR+and LR-),as well as the diagnostic odds ratio(DOR),and their 95%confidence intervals.We conducted subgroup analyses based on urea dosing,time after urea administration,and assessment technique.To investigate a possible threshold effect,we conducted Spearman correlation analysis,and we generated summary receiver operating characteristic(SROC)curves to assess heterogeneity.Finally,we visually inspected a funnel plot and used Egger’s test to evaluate publication bias.endorsing both as reliable diagnostic tools in clinical practice.CONCLUSION In summary,our study has demonstrated that ^(13)C-UBT has been found to outperform the ^(14)C-UBT,making it the preferred diagnostic approach.Additionally,our results emphasize the significance of carefully considering urea dosage,assessment timing,and measurement techniques for both tests to enhance diagnostic precision.Nevertheless,it is crucial for researchers and clinicians to evaluate the strengths and limitations of our findings before implementing them in practice.
基金supported by Fundamental Research Funds for the Central Universities(B220202062)supported by Key Program of National Natural Science Foundation of China(92047201,92047303,52102237)+1 种基金National Science Funds for Creative Research Groups of China(51421006)supported by Postdoctoral Science Foundations of China and Jiangsu Province(2021M690861,2022T150183,2021K065A)。
文摘Urea oxidation reaction(UOR)is proposed as an exemplary half-reaction in renewable energy applications because of its low thermodynamical potential.However,challenges persist due to sluggish reaction kinetics and complex by-products separation.To this end,we introduce the lattice oxygen oxidation mechanism(LOM),propelling a novel UOR route using a modified CoFe layered double hydroxide(LDH)catalyst termed CFRO-7.Theoretical calculations and in-situ characterizations highlight the activated lattice oxygen(O_(L))within CFRO-7 as pivotal sites for UOR,optimizing the reaction pathway and accelerating the kinetics.For the urea overall electrolysis application,the LOM route only requires a low voltage of 1.54 V to offer a high current of 100 mA cm^(-2) for long-term utilization(>48 h).Importantly,the by-product NCO^(-)−is significantly suppressed,while the CO_(2)2/N_(2) separation is efficiently achieved.This work proposed a pioneering paradigm,invoking the LOM pathway in urea electrolysis to expedite reaction dynamics and enhance product selectivity.
文摘In this editorial,we discuss the article in the World Journal of Gastroenterology.The article conducts a meta-analysis of the diagnostic accuracy of the urea breath test(UBT),a non-invasive method for detecting Helicobacter pylori(H.pylori)infection in humans.It is based on radionuclide-labeled urea.Various methods,both invasive and non-invasive,are available for diagnosing H.pylori infection,inclu-ding endoscopy with biopsy,serology for immunoglobulin titers,stool antigen analysis,and UBT.Several guidelines recommend UBTs as the primary choice for diagnosing H.pylori infection and for reexamining after eradication therapy.It is used to be the first choice non-invasive test due to their high accuracy,specificity,rapid results,and simplicity.Moreover,its performance remains unaffected by the distribution of H.pylori in the stomach,allowing a high flow of patients to be tested.Despite its widespread use,the performance characteristics of UBT have been inconsistently described and remain incompletely defined.There are two UBTs available with Food and Drug Administration approval:The 13C and 14C tests.Both tests are affordable and can provide real-time results.Physicians may prefer the 13C test because it is non-radioactive,compared to 14C which uses a radioactive isotope,especially in young children and pregnant women.Although there was heterogeneity among the studies regarding the diagnostic accuracy of both UBTs,13C-UBT consistently outperforms the 14C-UBT.This makes the 13C-UBT the preferred diagnostic approach.Furthermore,the provided findings of the meta-analysis emphasize the significance of precise considerations when choosing urea dosage,assessment timing,and measurement techniques for both the 13C-UBT and 14C-UBT,to enhance diagnostic precision.
基金support of the National Natural Science Foundation of China(21901246,22105203 and 22175174)the Natural Science Foundation of Fujian Province(2020J01116 and 2021J06033)the China Postdoctoral Science Foundation(2021TQ0332 and 2021M703215).
文摘Controllable design of the catalytic electrodes with hierarchical superstructures is expected to improve their electrochemical performance.Herein,a self-supported integrated electrode(NiCo-ZLDH/NF)with a unique hierarchical quaternary superstructure was fabricated through a self-sacrificing template strategy from the metal–organic framework(Co-ZIF-67)nanoplate arrays,which features an intriguing well-defined hierarchy when taking the unit cells of the NiCo-based layered double hydroxide(NiCo-LDH)as the primary structure,the ultrathin LDH nanoneedles as the secondary structure,the mesoscale hollow plates of the LDH nanoneedle arrays as the tertiary structure,and the macroscale three-dimensional frames of the plate arrays as the quaternary structure.Notably,the distinctive structure of NiCo-ZLDH/NF can not only accelerate both mass and charge transfer,but also expose plentiful accessible active sites with high intrinsic activity,endowing it with an excellent electrochemical performance for urea oxidation reaction(UOR).Specially,it only required the low potentials of 1.335,1.368 and 1.388 V to deliver the current densities of 10,100 and 200 mA cm^(-2),respectively,much superior to those for typical NiCo-LDH.Employing NiCo-ZLDH/NF as the bifunctional electrode for both anodic UOR and cathodic HER,an energy-saving electrolysis system was further explored which can greatly reduce the needed voltage of 213 mV to deliver the current density of 100 mA cm^(-2),as compared to the conventional water electrolysis system composed of OER.This work manifests that it is prospective to explore the hierarchically nanostructured electrodes and the innovative electrolytic technologies for high-efficiency electrocatalysis.
基金financially supported in China by Natural Science Funds for Distinguished Young Scholars of Heilongjiang Province(No.JC2018004)Natural Science Foundation of Heilongjiang Province of China(No.TD2020B001)in the USA by NSF-CREST Center for Innovation,Research,and Education in Environmental Nanotechnology(CIRE2N)(No.HRD-1736093)
文摘Urea synthesis through the simultaneous electrocatalytic reduction of N_(2)and CO_(2)molecules under ambient conditions holds great promises as a sustainable alternative to its industrial production,in which the development of stable,highly efficient,and highly selective catalysts to boost the chemisorption,activation,and coupling of inert N_(2)and CO_(2)molecules remains rather challenging.Herein,by means of density functional theory computations,we proposed a new class of two-dimensional nanomaterials,namely,transition-metal phosphide monolayers(TM_(2)P,TM=Ti,Fe,Zr,Mo,and W),as the potential electrocatalysts for urea production.Our results showed that these TM_(2)P materials exhibit outstanding stability and excellent metallic properties.Interestingly,the Mo_(2)P monolayer was screened out as the best catalyst for urea synthesis due to its small kinetic energy barrier(0.35 eV)for C-N coupling,low limiting potential(-0.39 V),and significant suppressing effects on the competing side reactions.The outstanding catalytic activity of the Mo_(2)P monolayer can be ascribed to its optimal adsorption strength with the key^(*)NCON species due to its moderate positive charges on the Mo active sites.Our findings not only propose a novel catalyst with high-efficiency and high-selectivity for urea production but also further widen the potential applications of metal phosphides in electrocatalysis.
基金National Natural Science Foundation of China (No. 22202065, 22075092 and U21A20500)。
文摘Urea is widely used as fertilizer and is a key substance supporting global food production. However, the traditional industrial synthesis of urea faces the challenges with high energy consumption and serious environmental problems. With the increasing global demand for environmental protection and sustainable development, it is much necessary to develop novel and clean methods for the synthesis of urea.Electrocatalysis provides an efficient and renewable synthesis route that can directly produce urea at room temperature and atmospheric pressure by the coupling of CO_(2) and nitrogenous molecules. In this review, we summarized the most recent advances in electrochemical synthesis of urea via CAN coupling systematically, focusing on the coupling of CO_(2) and different nitrogen sources. And the associated coupling mechanism, catalysts optimization, and electrolyzer design are well discussed. Moreover, the challenges and future directions for electrocatalytic CAN coupling are prospected. This review will provide timely and valuable guidance for others and attract more interests to promote the development of electrochemical synthesis of urea or other valuable chemicals containing CAN bond.
基金This work was supported by the National Key R&D Program of China(2021YFD1900700)the National Natural Science Foundation of China(52179046).
文摘The combined effects of straw incorporation(SI)and polymer-coated urea(PCU)application on soil ammonia(NH_(3))and nitrous oxide(N_(2)O)emissions from agricultural fields have not been comprehensively evaluated in Northwest China.We conducted a two-year field experiment to assess the effects of combining SI with either uncoated urea(U)or PCU on soil NH_(3)emissions,N_(2)O emissions,winter wheat yields,yield-scaled NH_(3)(/NH_(3)),and yield-scaled N_(2)O(/N_(2)O).Five treatments were investigated,no nitrogen(N)fertilizer(N_(0)),U application at 150 kg N ha-1 with and without SI(SI+U and S_(0)+U),and PCU application at 150 kg N ha^(-1) with and without SI(SI+PCU and S_(0)+PCU).The results showed that the NH_(3);emissions increased by 20.98-34.35%following Sl compared to straw removal,mainly due to increases in soil ammonium(NH_(4)^(+)-N)content and water-flled pore space(WFPS).SI resulted in higher N_(2)O emissions than under the So scenario by 13.31-49.23%due to increases in soil inorganic N(SIN)contents,WFPS,and soil microbial biomass.In contrast,the PCU application reduced the SIN contents compared to the U application,reducing the NH_(3)and N_(2)O emissions by 45.99-58.07 and 18.08-53.04%,respectively.Moreover,no significant positive effects of the SI or PCU applications on the winter wheat yield were observed.The lowest /NH_(3) and /N_(2)O values were observed under the S_(0)+PCU and SI+PCU treatments.Our results suggest that single PCU applications and their combination with straw are the optimal agricultural strategies for mitigating gaseous N emissions and maintaining optimal winter wheat yields in Northwest China.
文摘Metabolic reprogramming is a key feature driving oncogenesis in cancers. Recent studies have revealed that protein metabolism is largely altered in gliomas facilitating its malignant growth. Urea is the end product of nitrogen metabolism which is mainly produced by arginase. The interdependence of arginase and other biochemical mechanisms triggered scientific research interest. This research aimed to investigate the relationships between the urea as the main parameter of protein metabolism and glioma progression. It was also the most pronounced relationship between urea and the level of the nuclear protein Ki-67 as a marker of proliferative activity and O-6-methylguanine-DNA methyltransferase (MGMT), which performs DNA repair. Postoperative material from 20 patients with gliomas of different grades of anaplasia was analyzed.
