Water scarcity is a global challenge,and solar evaporation technology offers a promising and eco-friendly solution for freshwater production.Photothermal conversion materials(PCMs)are crucial for solar evaporation.Imp...Water scarcity is a global challenge,and solar evaporation technology offers a promising and eco-friendly solution for freshwater production.Photothermal conversion materials(PCMs)are crucial for solar evaporation.Improving photothermal conversion efficiency and reducing water evaporation enthalpy are the two key strategies for the designing of PCMs.The desired PCMs that combine both of these properties remain a challenging task,even with the latest advancements in the field.Herein,we developed copper nanoparticles(NPs)with different conjugated nitrogen-doped microporous carbon coatings(Cu@C–N)as PCMs.The microporous carbon enveloping layer provides a highly efficient pathway for water transport and a nanoconfined environment that protects Cu NPs and facilitates the evaporation of water clusters,reducing the enthalpy of water evaporation.Meanwhile,the conjugated nitrogen nodes form strong metal-organic coordination bonds with the surface of copper NPs,acting as an energy bridge to achieve rapid energy transfer and provide high solar-to-vapor conversion efficiency.The Cu@C–N exhibited up to 89.4%solar-to-vapor conversion efficiency and an evaporation rate of 1.94 kgm^(−2) h^(−1) under one sun irradiation,outperforming conventional PCMs,including carbon-based materials and semiconductor materials.These findings offer an efficient design scheme for high-performance PCMs essential for solar evaporators to address global water scarcity.展开更多
Objective:To analyze the impact of comprehensive rehabilitation therapy of traditional Chinese medicine(TCM)(based on modern rehabilitation training)on the spasticity and motor function in stroke patients with hemiple...Objective:To analyze the impact of comprehensive rehabilitation therapy of traditional Chinese medicine(TCM)(based on modern rehabilitation training)on the spasticity and motor function in stroke patients with hemiplegia.Methods:Seventy-nine stroke and hemiplegia patients admitted to the hospital from June 2021 to June 2023 were selected and randomly divided into a control group(39 cases)using modern rehabilitation training,and an observation group combined with comprehensive TCM rehabilitation therapy(40 cases),over 1 month.The clinical index data of the two groups were compared.Results:There were differences in the clinical index data between the two groups.The total effective rate after 2 treatment in the observation group(92.50%)was higher than that of the control group(74.36%)(χ^(2)=4.727,P<0.05).All central sensitization inventory(CSI)and stroke quality of life(PRO)scores in both groups were lower after treatment,with the observation group having lower scores as compared to the control group(P<0.05).The scores of FMA(upper limbs,lower limbs),Barthel index scores,and Functional Ambulation Categories(FAC)scores of both groups increased after treatment,with the observation group having higher scores as compared to the control group(P<0.05).Conclusion:Comprehensive TCM rehabilitation therapy had a significant therapeutic effect on patients with hemiplegia after stroke.It improved the patient’s spasticity,limb movement,and walking function.Their daily living abilities and quality of life were also enhanced.展开更多
探索非贵金属材料作为高效氧还原反应催化剂是迫切需要的,但具有一定的挑战性。本文采用等离子体轰击和酸洗相结合的策略合成了Co原子团簇修饰的多孔碳载体催化剂(CoAC/NC)。通过多种表征手段证实了的原子团簇特征。所得到的CoAC/NC催...探索非贵金属材料作为高效氧还原反应催化剂是迫切需要的,但具有一定的挑战性。本文采用等离子体轰击和酸洗相结合的策略合成了Co原子团簇修饰的多孔碳载体催化剂(CoAC/NC)。通过多种表征手段证实了的原子团簇特征。所得到的CoAC/NC催化剂在三电极体系和锌-空电池方面都表现出优异的氧还原反应活性。该催化剂的氧还原反应半波电位为0.887 V,显著优于商业Pt/C催化剂,且表现出优异的稳定性。此外,该催化剂组装的锌-空电池的峰值功率密度为181.5 m W·cm^(-2),同样远高于Pt/C催化剂。这项工作不仅合成了一种高效的氧还原反应催化剂,而且为原子团簇催化剂的理性设计和实际应用提供了新的见解。展开更多
Parts with high-quality freeform surfaces have been widely used in industries,which require strict quality control during the manufacturing process.Among all the industrial inspection methods,contact measurement with ...Parts with high-quality freeform surfaces have been widely used in industries,which require strict quality control during the manufacturing process.Among all the industrial inspection methods,contact measurement with coordinate measuring machines or computer numerical control machine tool is a fundamental technique due to its high accuracy,robustness,and universality.In this paper,the existing research in the contact measurement field is systematically reviewed.First,different configurations of the measuring machines are introduced in detail,which may have influence on the corresponding sampling and inspection path generation criteria.Then,the entire inspection pipeline is divided into two stages,namely the pre-inspection and post-inspection stages.The typical methods of each sub-stage are systematically overviewed and classified,including sampling,accessibility analysis,inspection path generation,probe tip radius compensation,surface reconstruction,and uncertainty analysis.Apart from those classical research,the applications of the emerging deep learning technique in some specific tasks of measurement are introduced.Furthermore,some potential and promising trends are provided for future investigation.展开更多
As a carbon-free energy carrier,hydrogen has become the pivot for future clean energy,while efficient hydrogen production and combustion still require precious metal-based catalysts.Single-atom catalysts(SACs)with hig...As a carbon-free energy carrier,hydrogen has become the pivot for future clean energy,while efficient hydrogen production and combustion still require precious metal-based catalysts.Single-atom catalysts(SACs)with high atomic utilization open up a desirable perspective for the scale applications of precious metals,but the general and facile preparation of various precious metal-based SACs remains challenging.Herein,a general movable printing method has been developed to synthesize various precious metal-based SACs,such as Pd,Pt,Rh,Ir,and Ru,and the features of highly dispersed single atoms with nitrogen coordination have been identified by comprehensive characterizations.More importantly,the synthesized Pt-and Ru-based SACs exhibit much higher activities than their corresponding nanoparticle counterparts for hydrogen oxidation reaction and hydrogen evolution reaction(HER).In addition,the Pd-based SAC delivers an excellent activity for photocatalytic hydrogen evolution.Especially for the superior mass activity of Ru-based SACs toward HER,density functional theory calculations confirmed that the adsorption of the hydrogen atom has a significant effect on the spin state and electronic structure of the catalysts.展开更多
Oxygen reduction reaction(ORR)is the heart of many new energy conversions and storage devices,such as metal-air batteries and fuel cells.However,ORR is currently facing the dilemma of sluggish intrinsic kinetics and t...Oxygen reduction reaction(ORR)is the heart of many new energy conversions and storage devices,such as metal-air batteries and fuel cells.However,ORR is currently facing the dilemma of sluggish intrinsic kinetics and the noble electrocatalysts of high price and low reserves.In this work,isolated Co atoms anchored on defective nitrogen-doped carbon graphene single-atom catalyst(Co-SAC/NC)are synthesized via the proposed movable type printing method.The prepared Co-SAC/NC catalyst demonstrates admirable ORR performance,with a high half-wave potential of 0.884 V in alkaline electrolytes and outstanding durability.In addition,an assembled zinc–air battery with prepared Co-SAC/NC as air-cathode catalyst displays a high-peak power density of 179 mW cm^(-2)and a high-specific capacity(757 mAh g^(-1)).Density functional theory calculations confirm that the true active sites of the prepared catalyst are Co-N_(4)moieties,and further reveal a significantly electronic structure evolution of Co sites in the ORR process,in which the project density of states and local magnetic moment of Co atom varies during its whole reaction process.This work not only paves a new avenue for synthesizing SACs as robust electrocatalysts,but also provides an electronic-level insight into the evolution of the electronic structure of single-atom catalysts.展开更多
Electrocatalytic CO_(2) reduction reaction(eCO_(2) RR)has significant relevance to settle the global energy crisis and abnormal climate problem via mitigating the excess emission of waste CO_(2) and producing high-val...Electrocatalytic CO_(2) reduction reaction(eCO_(2) RR)has significant relevance to settle the global energy crisis and abnormal climate problem via mitigating the excess emission of waste CO_(2) and producing high-value-added chemicals.Currently,eCO_(2) RR to formic acid or formate is one of the most technologically and economically viable approaches to realize high-efficiency CO_(2) utilization,and the development of efficient electrocatalysts is very urgent to achieve efficient and stable catalytic performance.In this review,the recent advances for two-dimensional bismuth-based nanosheets(2D Bi-based NSs)electrocatalysts are concluded from both theoretical and experimental perspectives.Firstly,the preparation strategies of 2D Bi-based NSs in aspects to precisely control the thickness and uniformity are summarized.In addition,the electronic regulation strategies of 2D Bi-based NSs are highlighted to gain insight into the effects of the structure-property relationship on facilitating CO_(2) activation,improving product selectivity,and optimizing carrier transport dynamics.Finally,the considerable challenges and opportunities of 2D Bi-based NSs are discussed to lighten new directions for future research of eCO_(2) RR.展开更多
The investigation of highly effective,durable,and cost-effective electrocatalysts for the hydrogen evolution reaction(HER)is a prerequisite for the upcoming hydrogen energy society.To establish a new hydrogen energy s...The investigation of highly effective,durable,and cost-effective electrocatalysts for the hydrogen evolution reaction(HER)is a prerequisite for the upcoming hydrogen energy society.To establish a new hydrogen energy system and gradually replace the traditional fossil-based energy,electrochemical water-splitting is considered the most promising,environmentally friendly,and efficient way to produce pure hydrogen.Compared with the commonly used platinum(Pt)-based catalysts,ruthenium(Ru)is expected to be a good alternative because of its similar hydrogen bonding energy,lower water decomposition barrier,and considerably lower price.Analyzing and revealing the HER mechanisms,as well as identifying a rational design of Ru-based HER catalysts with desirable activity and stability is indispensable.In this review,the research progress on HER electrocatalysts and the relevant describing parameters for HER performance are briefly introduced.Moreover,four major strategies to improve the performance of Ru-based electrocatalysts,including electronic effect modulation,support engineering,structure design,and maximum utilization(single atom)are discussed.Finally,the challenges,solutions and prospects are highlighted to prompt the practical applications of Rubased electrocatalysts for HER.展开更多
Exploring effective, durable, and affordable electrocatalysts of methanol oxidation reaction(MOR) is of vital significance for the industrial application of direct methanol fuel cells. Herein, an efficient, general,an...Exploring effective, durable, and affordable electrocatalysts of methanol oxidation reaction(MOR) is of vital significance for the industrial application of direct methanol fuel cells. Herein, an efficient, general,and expandable method is developed to synthesis two-dimensional(2D) ternary Pt Bi M nanoplates(NPLs), in which various M(Co, Ni, Cu, Zn, Sn) is severed as the third component to the binary Pt Bi system. The MOR performance of Pt Bi M NPLs is entirely investigated, demonstrating that both the MOR activity and durability is enhanced with the introduction of the additional composition. Pt3Bi3Zn NPLs shows much higher MOR activity and stability than that of the Pt Bi counterparts, not to mention the current advanced Pt Ru/C and Pt/C catalysts. The prominent performances are attributed to the modulated electronic structure of the surface Pt in Pt Bi NPLs by the addition of Zn, resulting in a weakened affination between Pt and the adsorbed poisoning species(mainly CO) compared with Pt Bi NPLs, verified by density functional theory(DFT) calculations. In addition, the absorbed OH can be generated on the surface of Zn atom due to its favorable water activation properties, thus the CO removal on the adjacent Pt atoms is accelerated, further leading to a high activity and anti-poisoning performance of the resulting Pt_(3)Bi_(3)Zn catalyst. This work provides new insights and robust strategy for highly efficient MOR electrocatalyst with extraordinary anti-poisoning performance and stability.展开更多
Objective:To investigate oncological outcomes in patients with bladder cancer who underwent minimally invasive radical cystectomy(MIRC)or open radical cystectomy(ORC).Methods:We identified patients with bladder cancer...Objective:To investigate oncological outcomes in patients with bladder cancer who underwent minimally invasive radical cystectomy(MIRC)or open radical cystectomy(ORC).Methods:We identified patients with bladder cancer who underwent radical cystectomy(RC)in 13 centers of the Chinese Bladder Cancer Consortium(CBCC).Perioperative outcomes were compared between MIRC and ORC.The influence of surgical approaches on overall survival(OS)and cancer-specific survival(CSS)in the entire study group and subgroups classified according to pathologic stage or lymph node(LN)status was assessed with the log-rank test.Multivariable Cox proportional hazard models were used to evaluate the association among OS,CSS and risk factors of interest.Results:Of 2098 patients who underwent RC,1243 patients underwent MIRC(1087 laparoscopic RC and 156 robotic-assisted RC,respectively),while 855 patients underwent ORC.No significant differences were noted in positive surgical margin rate and 90-day postoperative mortality rate.MIRC was associated with less estimated blood loss,more LN yield,higher rate of neobladder diversion,longer operative time,and longer length of hospital stay.There was no significant difference in OS and CSS according to surgical approaches(pZ0.653,and 0.816,respectively).Subgroup analysis revealed that OS and CSS were not significantly different regardless of the status of extravesical involvement or LN involvement.Multivariable Cox regression analyses showed that the surgical approach was not a significant predictor of OS and CSS.Conclusions:Our study showed that MIRC was comparable to conventional ORC in terms of OS and CSS.展开更多
Integration of electronic and strain effects with tailored structures is significant to tuning the electrocatalytic activity and stability of the electrocatalysts for the oxygen reduction reaction(ORR).In this study,o...Integration of electronic and strain effects with tailored structures is significant to tuning the electrocatalytic activity and stability of the electrocatalysts for the oxygen reduction reaction(ORR).In this study,onedimensional PtFe hollow nanochains are synthesized by a facile and effective method,which exhibit a highly open and porous structure.The modulated electronic and strain effects of Pt atoms are verified by extensive structural characterizations,and the mass and specific activities of the prepared catalyst are roughly 7.45 and 12.44 times higher than those of the commercial Pt/C catalyst,respectively.Remarkably,the catalyst demonstrates robust performance with negligible activity decay after an accelerated durability test for 30,000 cycles.The high activity of the catalyst is probably due to the optimized absorption affinity of Pt-O accelerating the reaction kinetics induced by the cooperation of Fe atoms as well as the unique hollow and curved structures.This study provides new insights into the rational design of high-performance ORR catalysts with considerable durability.展开更多
High-efficiency photocatalytic hydrogen evolution(PHE)relies on the development of inexpensive,stable,and efficient photocatalysts.Cadmium sulfide(CdS),as a typical binary metal sulfide,has attracted considerable rese...High-efficiency photocatalytic hydrogen evolution(PHE)relies on the development of inexpensive,stable,and efficient photocatalysts.Cadmium sulfide(CdS),as a typical binary metal sulfide,has attracted considerable research attention due to its negative conduction band position,narrow band gap for visible-light response,and strong driving force for PHE.However,the construction of CdSbased photocatalysts and the PHE rate still require improvement for practical applications.In this review,recent advances in CdS-based photocatalysts for PHE via water splitting are systematically summarized.First,the semiconductor properties of CdS,including the crystal and band structures,are briefly introduced.Afterward,the fundamental mechanisms of PHE using semiconductor photocatalysts via water splitting are discussed.Subsequently,the photoactivity of bare CdS with different morphologies and structures,CdS with cocatalyst loading,and CdS-based heterojunction photocatalysts are reviewed and discussed in detail.Finally,the challenges and prospects for exploring advanced CdS-based photocatalysts are provided.展开更多
直接乙醇燃料电池(DEFCs)被认为是最有前途的便携式电源设备之一.目前用于DEFCs的主流催化剂是Pt基或Pd基催化剂,然而它们不能有效地断裂C–C键,只能使乙醇部分氧化为CH_(3)CHO或CH_(3)COOH.此外,大多数贵金属催化剂容易被反应中间体CO...直接乙醇燃料电池(DEFCs)被认为是最有前途的便携式电源设备之一.目前用于DEFCs的主流催化剂是Pt基或Pd基催化剂,然而它们不能有效地断裂C–C键,只能使乙醇部分氧化为CH_(3)CHO或CH_(3)COOH.此外,大多数贵金属催化剂容易被反应中间体CO毒化,降低了催化剂的稳定性和寿命,这些因素都抑制了催化剂的实际应用.本文中,我们报道了一种用于乙醇氧化反应的具有不同Rh含量的超细三金属PtNiRh纳米线,Pt_(6)Ni_(2)Rh_(3)/C具有最优的催化活性(1.16 A mg_(Pt^(-1)))、抗CO中毒能力和稳定性.理论计算表明,在双金属PtNi中引入Rh,使得该催化剂具有良好的中间物吸附和C–C键断裂能力,有利于乙醇的完全氧化.展开更多
Excitonic confinement greatly determines the charge carrier transport of photocatalysts.A molten salt modulation of excitonic con-finement is herein demonstrated as formation of ultrafine carbon-doped anatase TiO_(2)w...Excitonic confinement greatly determines the charge carrier transport of photocatalysts.A molten salt modulation of excitonic con-finement is herein demonstrated as formation of ultrafine carbon-doped anatase TiO_(2)with grafted graphitic carbon nitride,which is rationalized as an excellent catalyst for overall CO_(2)photoreduction.Compared with bulk TiO_(2),the carbon-doped TiO_(2)(M-TiO_(2))pos-sesses a weaker excitonic confinement to decrease exciton binding energy from 99 to 58 meV,consequently enhancing free-charge-carrier generation and transportation.Effective Z-scheme electron transfer from M-TiO_(2)to C_(3)N_(4) is built,enhancing the CO_(2)conversion via the synchronous optimization of redox ability,CO_(2)activation,and^(*)COOH generation.This work highlights the unique chemistry of excitonic dissociation on facilitating separation of electron and hole,and also extends the scope of molten salt-mediated modulation of photocatalysis materials.展开更多
Robust oxygen reduction reaction(ORR)catalysts are essential for energy storage and conversion devices,but their development remains challenging.Herein,we design a single-atom catalyst featuring isolated Co anchored o...Robust oxygen reduction reaction(ORR)catalysts are essential for energy storage and conversion devices,but their development remains challenging.Herein,we design a single-atom catalyst featuring isolated Co anchored on nitrogen-doped carbon(Co-SAC/NC)via a highly efficient“plasma-bombing”strategy.With a high loading(up to 2.5wt%),the well-dispersed single Co atoms in Co-SAC/NC give it robust ORR performance in an alkaline medium.It also demonstrates excellent battery performance when implemented as the air-cathode catalyst in a zinc-air battery(ZAB).Theoretical calculations reveal that the Co-N_(4)moiety experiences an“extraction/recovery”structural evolution during the ORR process,and the reaction's rate-determining step is the formation of OOH∗(reaction intermediate).This work provides a new strategy for designing robust ORR catalysts for high-performance ZABs and other energy-conversion devices.展开更多
The structure of parabolic condensers makes them susceptible to wind load because of their thin and large windward mirrors.In this paper,the wind pressure on a model of a condenser mirror(1:35)on multistorey flat roof...The structure of parabolic condensers makes them susceptible to wind load because of their thin and large windward mirrors.In this paper,the wind pressure on a model of a condenser mirror(1:35)on multistorey flat roofs is analysed via pressure measurement in a wind tunnel.The mean wind-pressure distribution law of flat-roof condenser mirrors(including the change law with working conditions and the maximum distribution characteristics)and the distribution law of fluctuating and extreme wind pressure are obtained.Furthermore,by comparison with the ground-based condenser distribution law,similarities and differences between the two are obtained.Research results show that the wind-pressure distribution law of flat-roof parabolic condenser mirrors is the same as those on the ground,but the mean wind-pressure coefficient(absolute value)is generally~30%smaller.Furthermore,the maximum effect is generally located at the windward mirror edge and the mirror is more susceptible to wind pressure in wind directions of 30°and 135°-150°.The results of this study can provide a theoretical reference for wind-resistant structure design and multistorey flat-roof condenser-related research.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.52162012,52262014,22368019)Key Research and Development Project of Hainan Province(Grant Nos.ZDYF2022SHFZ053,ZDYF2021GXJS209)+1 种基金Science and Technology Innovation Talent Platform Fund for South China Sea New Star of Hainan Province(Grant No.NHXXRCXM202305)Open Research Project of State Key Laboratory of Marine Resource Utilization in South China Sea(Grant No.MRUKF2023020).
文摘Water scarcity is a global challenge,and solar evaporation technology offers a promising and eco-friendly solution for freshwater production.Photothermal conversion materials(PCMs)are crucial for solar evaporation.Improving photothermal conversion efficiency and reducing water evaporation enthalpy are the two key strategies for the designing of PCMs.The desired PCMs that combine both of these properties remain a challenging task,even with the latest advancements in the field.Herein,we developed copper nanoparticles(NPs)with different conjugated nitrogen-doped microporous carbon coatings(Cu@C–N)as PCMs.The microporous carbon enveloping layer provides a highly efficient pathway for water transport and a nanoconfined environment that protects Cu NPs and facilitates the evaporation of water clusters,reducing the enthalpy of water evaporation.Meanwhile,the conjugated nitrogen nodes form strong metal-organic coordination bonds with the surface of copper NPs,acting as an energy bridge to achieve rapid energy transfer and provide high solar-to-vapor conversion efficiency.The Cu@C–N exhibited up to 89.4%solar-to-vapor conversion efficiency and an evaporation rate of 1.94 kgm^(−2) h^(−1) under one sun irradiation,outperforming conventional PCMs,including carbon-based materials and semiconductor materials.These findings offer an efficient design scheme for high-performance PCMs essential for solar evaporators to address global water scarcity.
文摘Objective:To analyze the impact of comprehensive rehabilitation therapy of traditional Chinese medicine(TCM)(based on modern rehabilitation training)on the spasticity and motor function in stroke patients with hemiplegia.Methods:Seventy-nine stroke and hemiplegia patients admitted to the hospital from June 2021 to June 2023 were selected and randomly divided into a control group(39 cases)using modern rehabilitation training,and an observation group combined with comprehensive TCM rehabilitation therapy(40 cases),over 1 month.The clinical index data of the two groups were compared.Results:There were differences in the clinical index data between the two groups.The total effective rate after 2 treatment in the observation group(92.50%)was higher than that of the control group(74.36%)(χ^(2)=4.727,P<0.05).All central sensitization inventory(CSI)and stroke quality of life(PRO)scores in both groups were lower after treatment,with the observation group having lower scores as compared to the control group(P<0.05).The scores of FMA(upper limbs,lower limbs),Barthel index scores,and Functional Ambulation Categories(FAC)scores of both groups increased after treatment,with the observation group having higher scores as compared to the control group(P<0.05).Conclusion:Comprehensive TCM rehabilitation therapy had a significant therapeutic effect on patients with hemiplegia after stroke.It improved the patient’s spasticity,limb movement,and walking function.Their daily living abilities and quality of life were also enhanced.
文摘探索非贵金属材料作为高效氧还原反应催化剂是迫切需要的,但具有一定的挑战性。本文采用等离子体轰击和酸洗相结合的策略合成了Co原子团簇修饰的多孔碳载体催化剂(CoAC/NC)。通过多种表征手段证实了的原子团簇特征。所得到的CoAC/NC催化剂在三电极体系和锌-空电池方面都表现出优异的氧还原反应活性。该催化剂的氧还原反应半波电位为0.887 V,显著优于商业Pt/C催化剂,且表现出优异的稳定性。此外,该催化剂组装的锌-空电池的峰值功率密度为181.5 m W·cm^(-2),同样远高于Pt/C催化剂。这项工作不仅合成了一种高效的氧还原反应催化剂,而且为原子团簇催化剂的理性设计和实际应用提供了新的见解。
基金partially supported by the Natural Science Foundation of Shanghai(Grant No.22ZR1435200)the National Natural Science Foundation of China(Grant No.52075337)the Open Research Fund of State Key Laboratory of Digital Manufacturing and Equipment Technology,HUST(Grant No.DMETKF2022010)。
文摘Parts with high-quality freeform surfaces have been widely used in industries,which require strict quality control during the manufacturing process.Among all the industrial inspection methods,contact measurement with coordinate measuring machines or computer numerical control machine tool is a fundamental technique due to its high accuracy,robustness,and universality.In this paper,the existing research in the contact measurement field is systematically reviewed.First,different configurations of the measuring machines are introduced in detail,which may have influence on the corresponding sampling and inspection path generation criteria.Then,the entire inspection pipeline is divided into two stages,namely the pre-inspection and post-inspection stages.The typical methods of each sub-stage are systematically overviewed and classified,including sampling,accessibility analysis,inspection path generation,probe tip radius compensation,surface reconstruction,and uncertainty analysis.Apart from those classical research,the applications of the emerging deep learning technique in some specific tasks of measurement are introduced.Furthermore,some potential and promising trends are provided for future investigation.
基金National Natural Science Foundation of China,Grant/Award Numbers:62105083,22109034,22109035,52164028Start-up Research Foundation of Hainan University,Grant/Award Numbers:KYQD(ZR)-20008,KYQD(ZR)-20082,KYQD(ZR)-20083,KYQD(ZR)-20084,KYQD(ZR)-21065,KYQD(ZR)-21124,KYQD(ZR)-21125+4 种基金Basic and Applied Basic Research Foundation of Guangdong Province,Grant/Award Number:2019A1515110558Hainan Provincial Postdoctoral Science Foundation,Grant/Award Number:RZ2100007123Hainan Province Science and Technology Special Fund,Grant/Award Numbers:ZDYF2020037,ZDYF2020207Hainan Provincial Natural Science Foundation,Grant/Award Numbers:222MS009,222RC548The specific research fund of The Innovation Platform for Academicians of Hainan Province。
文摘As a carbon-free energy carrier,hydrogen has become the pivot for future clean energy,while efficient hydrogen production and combustion still require precious metal-based catalysts.Single-atom catalysts(SACs)with high atomic utilization open up a desirable perspective for the scale applications of precious metals,but the general and facile preparation of various precious metal-based SACs remains challenging.Herein,a general movable printing method has been developed to synthesize various precious metal-based SACs,such as Pd,Pt,Rh,Ir,and Ru,and the features of highly dispersed single atoms with nitrogen coordination have been identified by comprehensive characterizations.More importantly,the synthesized Pt-and Ru-based SACs exhibit much higher activities than their corresponding nanoparticle counterparts for hydrogen oxidation reaction and hydrogen evolution reaction(HER).In addition,the Pd-based SAC delivers an excellent activity for photocatalytic hydrogen evolution.Especially for the superior mass activity of Ru-based SACs toward HER,density functional theory calculations confirmed that the adsorption of the hydrogen atom has a significant effect on the spin state and electronic structure of the catalysts.
基金supported by the Hainan Province Science and Technology Special Fund(ZDYF2020037,2020207)the National Natural Science Foundation of China(21805104,22109034,22109035,52164028,62105083),the Postdoctoral Science Foundation of Hainan Province(RZ2100007123)the Start-up Research Foundation of Hainan University(KYQD(ZR)-20008,20082,20083,20084,21065,21124,21125).
文摘Oxygen reduction reaction(ORR)is the heart of many new energy conversions and storage devices,such as metal-air batteries and fuel cells.However,ORR is currently facing the dilemma of sluggish intrinsic kinetics and the noble electrocatalysts of high price and low reserves.In this work,isolated Co atoms anchored on defective nitrogen-doped carbon graphene single-atom catalyst(Co-SAC/NC)are synthesized via the proposed movable type printing method.The prepared Co-SAC/NC catalyst demonstrates admirable ORR performance,with a high half-wave potential of 0.884 V in alkaline electrolytes and outstanding durability.In addition,an assembled zinc–air battery with prepared Co-SAC/NC as air-cathode catalyst displays a high-peak power density of 179 mW cm^(-2)and a high-specific capacity(757 mAh g^(-1)).Density functional theory calculations confirm that the true active sites of the prepared catalyst are Co-N_(4)moieties,and further reveal a significantly electronic structure evolution of Co sites in the ORR process,in which the project density of states and local magnetic moment of Co atom varies during its whole reaction process.This work not only paves a new avenue for synthesizing SACs as robust electrocatalysts,but also provides an electronic-level insight into the evolution of the electronic structure of single-atom catalysts.
基金supported by the Hainan Provincial Natural Science Foundation of China(222RC548)the National Natural Science Foun-dation of China(22109034,22109035,52164028,62105083,21805104)+3 种基金the Opening Project of Key Laboratory of Electrochemical Energy Storage and Energy Conversion of Hainan Province(KFKT2021007)the Start-up Research Foundation of Hainan University(KYQD(ZR)-20008,20082,20083,20084,21065,21124,21125)the Innovative Research Projects for Graduate Students of Hainan Province(Qhyb2022-89,Qhys2022-174)the State Key Laboratory of Powder Metallurgy,Central South University,Changsha,China and the Specific Research Fund of the Innovation Platform for Academicians of Hainan Province.
文摘Electrocatalytic CO_(2) reduction reaction(eCO_(2) RR)has significant relevance to settle the global energy crisis and abnormal climate problem via mitigating the excess emission of waste CO_(2) and producing high-value-added chemicals.Currently,eCO_(2) RR to formic acid or formate is one of the most technologically and economically viable approaches to realize high-efficiency CO_(2) utilization,and the development of efficient electrocatalysts is very urgent to achieve efficient and stable catalytic performance.In this review,the recent advances for two-dimensional bismuth-based nanosheets(2D Bi-based NSs)electrocatalysts are concluded from both theoretical and experimental perspectives.Firstly,the preparation strategies of 2D Bi-based NSs in aspects to precisely control the thickness and uniformity are summarized.In addition,the electronic regulation strategies of 2D Bi-based NSs are highlighted to gain insight into the effects of the structure-property relationship on facilitating CO_(2) activation,improving product selectivity,and optimizing carrier transport dynamics.Finally,the considerable challenges and opportunities of 2D Bi-based NSs are discussed to lighten new directions for future research of eCO_(2) RR.
基金supported by the Key Research and Development Project of Hainan Province(ZDYF2020037,ZDYF2020207)the National Natural Science Foundation of China(21805104)+1 种基金Innovative Research Projects for Graduate Students of Hainan Province(Hyb2020-05)the Start-up Research Foundation of Hainan University(KYQD(ZR)-20008,20083,20084)。
文摘The investigation of highly effective,durable,and cost-effective electrocatalysts for the hydrogen evolution reaction(HER)is a prerequisite for the upcoming hydrogen energy society.To establish a new hydrogen energy system and gradually replace the traditional fossil-based energy,electrochemical water-splitting is considered the most promising,environmentally friendly,and efficient way to produce pure hydrogen.Compared with the commonly used platinum(Pt)-based catalysts,ruthenium(Ru)is expected to be a good alternative because of its similar hydrogen bonding energy,lower water decomposition barrier,and considerably lower price.Analyzing and revealing the HER mechanisms,as well as identifying a rational design of Ru-based HER catalysts with desirable activity and stability is indispensable.In this review,the research progress on HER electrocatalysts and the relevant describing parameters for HER performance are briefly introduced.Moreover,four major strategies to improve the performance of Ru-based electrocatalysts,including electronic effect modulation,support engineering,structure design,and maximum utilization(single atom)are discussed.Finally,the challenges,solutions and prospects are highlighted to prompt the practical applications of Rubased electrocatalysts for HER.
基金supported by the Hainan Province Science and Technology Special Fund(ZDYF2020037,2020207)the National Natural Science Foundation of China(21805104,22109034,22109035,52164028,62105083)+3 种基金the Basic and Applied Basic Research Foundation of Guangdong Province(2019A1515110558)the Research Fund Program of Key Laboratory of Fuel Cell Technology of Guangdong Province(202021)the Innovative Research Projects for Graduate Students of Hainan Province(Qhys2021-134)the Start-up Research Foundation of Hainan University(KYQD(ZR)-20008,20082,20083,20084,21065,21124,21125)。
文摘Exploring effective, durable, and affordable electrocatalysts of methanol oxidation reaction(MOR) is of vital significance for the industrial application of direct methanol fuel cells. Herein, an efficient, general,and expandable method is developed to synthesis two-dimensional(2D) ternary Pt Bi M nanoplates(NPLs), in which various M(Co, Ni, Cu, Zn, Sn) is severed as the third component to the binary Pt Bi system. The MOR performance of Pt Bi M NPLs is entirely investigated, demonstrating that both the MOR activity and durability is enhanced with the introduction of the additional composition. Pt3Bi3Zn NPLs shows much higher MOR activity and stability than that of the Pt Bi counterparts, not to mention the current advanced Pt Ru/C and Pt/C catalysts. The prominent performances are attributed to the modulated electronic structure of the surface Pt in Pt Bi NPLs by the addition of Zn, resulting in a weakened affination between Pt and the adsorbed poisoning species(mainly CO) compared with Pt Bi NPLs, verified by density functional theory(DFT) calculations. In addition, the absorbed OH can be generated on the surface of Zn atom due to its favorable water activation properties, thus the CO removal on the adjacent Pt atoms is accelerated, further leading to a high activity and anti-poisoning performance of the resulting Pt_(3)Bi_(3)Zn catalyst. This work provides new insights and robust strategy for highly efficient MOR electrocatalyst with extraordinary anti-poisoning performance and stability.
基金supported by the National Natural Science Foundation of China(Grant No.81825016,81772719,81772728,81572514)the Key Areas Research and Development Program of Guangdong(Grant No.2018B010109006)Medical Scientific Research Foundation of Guangdong Province(Grant No.A2018388).
文摘Objective:To investigate oncological outcomes in patients with bladder cancer who underwent minimally invasive radical cystectomy(MIRC)or open radical cystectomy(ORC).Methods:We identified patients with bladder cancer who underwent radical cystectomy(RC)in 13 centers of the Chinese Bladder Cancer Consortium(CBCC).Perioperative outcomes were compared between MIRC and ORC.The influence of surgical approaches on overall survival(OS)and cancer-specific survival(CSS)in the entire study group and subgroups classified according to pathologic stage or lymph node(LN)status was assessed with the log-rank test.Multivariable Cox proportional hazard models were used to evaluate the association among OS,CSS and risk factors of interest.Results:Of 2098 patients who underwent RC,1243 patients underwent MIRC(1087 laparoscopic RC and 156 robotic-assisted RC,respectively),while 855 patients underwent ORC.No significant differences were noted in positive surgical margin rate and 90-day postoperative mortality rate.MIRC was associated with less estimated blood loss,more LN yield,higher rate of neobladder diversion,longer operative time,and longer length of hospital stay.There was no significant difference in OS and CSS according to surgical approaches(pZ0.653,and 0.816,respectively).Subgroup analysis revealed that OS and CSS were not significantly different regardless of the status of extravesical involvement or LN involvement.Multivariable Cox regression analyses showed that the surgical approach was not a significant predictor of OS and CSS.Conclusions:Our study showed that MIRC was comparable to conventional ORC in terms of OS and CSS.
基金National Natural Science Foundation of China,Grant/Award Numbers:22109034,22109035,52164028,62105083Hainan Province Science and Technology Special Fund,Grant/Award Numbers:ZDYF2020037,2020207+1 种基金Start-up Research Foundation of Hainan University,Grant/Award Numbers:KYQD(ZR)-20008,20082,20083,20084,21065,21124,21125Postdoctoral Science Foundation of Hainan Province,Grant/Award Number:RZ2100007123。
文摘Integration of electronic and strain effects with tailored structures is significant to tuning the electrocatalytic activity and stability of the electrocatalysts for the oxygen reduction reaction(ORR).In this study,onedimensional PtFe hollow nanochains are synthesized by a facile and effective method,which exhibit a highly open and porous structure.The modulated electronic and strain effects of Pt atoms are verified by extensive structural characterizations,and the mass and specific activities of the prepared catalyst are roughly 7.45 and 12.44 times higher than those of the commercial Pt/C catalyst,respectively.Remarkably,the catalyst demonstrates robust performance with negligible activity decay after an accelerated durability test for 30,000 cycles.The high activity of the catalyst is probably due to the optimized absorption affinity of Pt-O accelerating the reaction kinetics induced by the cooperation of Fe atoms as well as the unique hollow and curved structures.This study provides new insights into the rational design of high-performance ORR catalysts with considerable durability.
基金the Natural Science Foundation of Hainan Province(grant no.521RC495)the National Natural Science Foundation of China(grant nos.22109034,22109035,52164028,and 62105083)+1 种基金the Foundation of State Key Laboratory of Marine Resource Utilization in South China Sea(Hainan University,grant no.MRUKF2021029)the Start-up Research Foundation of Hainan University(grant nos.KYQD(ZR)-20008,20082,20083,20084,21065,21124,and 21125).
文摘High-efficiency photocatalytic hydrogen evolution(PHE)relies on the development of inexpensive,stable,and efficient photocatalysts.Cadmium sulfide(CdS),as a typical binary metal sulfide,has attracted considerable research attention due to its negative conduction band position,narrow band gap for visible-light response,and strong driving force for PHE.However,the construction of CdSbased photocatalysts and the PHE rate still require improvement for practical applications.In this review,recent advances in CdS-based photocatalysts for PHE via water splitting are systematically summarized.First,the semiconductor properties of CdS,including the crystal and band structures,are briefly introduced.Afterward,the fundamental mechanisms of PHE using semiconductor photocatalysts via water splitting are discussed.Subsequently,the photoactivity of bare CdS with different morphologies and structures,CdS with cocatalyst loading,and CdS-based heterojunction photocatalysts are reviewed and discussed in detail.Finally,the challenges and prospects for exploring advanced CdS-based photocatalysts are provided.
基金supported by Hainan Province Science and Technology Special Fund(ZDYF2021GXJS207,ZDYF2020037,and 2020207)the National Natural Science Foundation of China(22109034,22109035,52164028,and 62105083)+2 种基金the Foundation of State Key Laboratory of Marine Resource Utilization in South China Sea(Hainan University,MRUKF2021029)the specific research fund of the Innovation Platform for Academicians of Hainan Provincethe“Young Talent Support Plan”of Xi’an Jiaotong University。
文摘直接乙醇燃料电池(DEFCs)被认为是最有前途的便携式电源设备之一.目前用于DEFCs的主流催化剂是Pt基或Pd基催化剂,然而它们不能有效地断裂C–C键,只能使乙醇部分氧化为CH_(3)CHO或CH_(3)COOH.此外,大多数贵金属催化剂容易被反应中间体CO毒化,降低了催化剂的稳定性和寿命,这些因素都抑制了催化剂的实际应用.本文中,我们报道了一种用于乙醇氧化反应的具有不同Rh含量的超细三金属PtNiRh纳米线,Pt_(6)Ni_(2)Rh_(3)/C具有最优的催化活性(1.16 A mg_(Pt^(-1)))、抗CO中毒能力和稳定性.理论计算表明,在双金属PtNi中引入Rh,使得该催化剂具有良好的中间物吸附和C–C键断裂能力,有利于乙醇的完全氧化.
基金funding support from the National Natural Science Foundation of China(22272120,U2202251,92045302)the Fundamental Research Funds for the Central Universities(2042022kf1174,2042021kf0213)+1 种基金the Hainan Province Science and Technology Special Fund(ZDYF2021SHFZ058,ZDYF2020207)the High-level Talent Project of Hainan Natural Science Foundation(2019RC075).
文摘Excitonic confinement greatly determines the charge carrier transport of photocatalysts.A molten salt modulation of excitonic con-finement is herein demonstrated as formation of ultrafine carbon-doped anatase TiO_(2)with grafted graphitic carbon nitride,which is rationalized as an excellent catalyst for overall CO_(2)photoreduction.Compared with bulk TiO_(2),the carbon-doped TiO_(2)(M-TiO_(2))pos-sesses a weaker excitonic confinement to decrease exciton binding energy from 99 to 58 meV,consequently enhancing free-charge-carrier generation and transportation.Effective Z-scheme electron transfer from M-TiO_(2)to C_(3)N_(4) is built,enhancing the CO_(2)conversion via the synchronous optimization of redox ability,CO_(2)activation,and^(*)COOH generation.This work highlights the unique chemistry of excitonic dissociation on facilitating separation of electron and hole,and also extends the scope of molten salt-mediated modulation of photocatalysis materials.
基金This work was supported by the Hainan Provincial Natural Science Foundation of China(211RC1018)the National Natural Science Foundation of China(22109034,22109035,52164028,62105083)+2 种基金Hainan Province Science and Technology Special Fund(ZDYF2021GXJS207,ZDYF2020037,ZDYF2020207)Natural Science Foundation of Shaanxi Province(2020JZ-23)the Start-up Research Foundation of Hainan University((KYQD(ZR)-20008,20082,20083,20084,21065,21124,21125).Appendix A.Supplementary data。
文摘Robust oxygen reduction reaction(ORR)catalysts are essential for energy storage and conversion devices,but their development remains challenging.Herein,we design a single-atom catalyst featuring isolated Co anchored on nitrogen-doped carbon(Co-SAC/NC)via a highly efficient“plasma-bombing”strategy.With a high loading(up to 2.5wt%),the well-dispersed single Co atoms in Co-SAC/NC give it robust ORR performance in an alkaline medium.It also demonstrates excellent battery performance when implemented as the air-cathode catalyst in a zinc-air battery(ZAB).Theoretical calculations reveal that the Co-N_(4)moiety experiences an“extraction/recovery”structural evolution during the ORR process,and the reaction's rate-determining step is the formation of OOH∗(reaction intermediate).This work provides a new strategy for designing robust ORR catalysts for high-performance ZABs and other energy-conversion devices.
基金supported by National Natural Science Foundation of China(grant number:51708478)the Natural Science Foundation of Hunan province(grant number:2020JJ5549)the State Key Laboratory of Marine Resource Utilization in South China Sea(MRUKF2021028).
文摘The structure of parabolic condensers makes them susceptible to wind load because of their thin and large windward mirrors.In this paper,the wind pressure on a model of a condenser mirror(1:35)on multistorey flat roofs is analysed via pressure measurement in a wind tunnel.The mean wind-pressure distribution law of flat-roof condenser mirrors(including the change law with working conditions and the maximum distribution characteristics)and the distribution law of fluctuating and extreme wind pressure are obtained.Furthermore,by comparison with the ground-based condenser distribution law,similarities and differences between the two are obtained.Research results show that the wind-pressure distribution law of flat-roof parabolic condenser mirrors is the same as those on the ground,but the mean wind-pressure coefficient(absolute value)is generally~30%smaller.Furthermore,the maximum effect is generally located at the windward mirror edge and the mirror is more susceptible to wind pressure in wind directions of 30°and 135°-150°.The results of this study can provide a theoretical reference for wind-resistant structure design and multistorey flat-roof condenser-related research.
