Recently, significant oil discoveries have been made in the shallower pay zones of the Jurassic Badaowan Formation (J_(1)b) in the Mahu Sag, Junggar Basin, Northwest China. However, little work has been done on the ge...Recently, significant oil discoveries have been made in the shallower pay zones of the Jurassic Badaowan Formation (J_(1)b) in the Mahu Sag, Junggar Basin, Northwest China. However, little work has been done on the geochemical characteristics and origins of the oil in the J_(1)b reservoir. This study analyzes 44 oil and 14 source rock samples from the area in order to reveal their organic geochemical characteristics and the origins of the oils. The J_(1)b oils are characterized by a low Pr/Ph ratio and high β-carotene and gammacerane indices, which indicate that they were mainly generated from source rocks deposited in a hypersaline environment. The oils are also extremely enhanced in C_(29) regular steranes, possibly derived from halophilic algae. Oil-source correlation shows that the oils were derived from the Lower Permian Fengcheng Formation (P_(1)f) source rocks, which were deposited in a strongly stratified and highly saline water column with a predominance of algal/bacterial input in the organic matter. The source rocks of the Middle Permian lower-Wuerhe Formation (P_(2)w), which were deposited in fresh to slightly saline water conditions with a greater input of terrigenous organic matter, make only a minor contribution to the J_(1)b oils. The reconstruction of the oil accumulation process shows that the J_(1)b oil reservoir may have been twice charged during Late Jurassic–Early Cretaceous and the Paleogene–Neogene, respectively. A large amount volume of hydrocarbons generated in the P_(1)f source rock and leaked from T_(1)b oil reservoirs migrated along faults connecting source beds and shallow-buried secondary faults into Jurassic traps, resulting in large-scale accumulations in J_(1)b. These results are crucial for understanding the petroleum system of the Mahu Sag and will provide valuable guidance for petroleum exploration in the shallower formations in the slope area of the sag.展开更多
Spinel LiNi_(0.5)Mn_(1.5)O_(4)(LNMO),a 5 V class high voltage cathode,has been regarded as an attractive candidate to further improve the energy density of lithium-ion battery.The issue simultaneously enabling side st...Spinel LiNi_(0.5)Mn_(1.5)O_(4)(LNMO),a 5 V class high voltage cathode,has been regarded as an attractive candidate to further improve the energy density of lithium-ion battery.The issue simultaneously enabling side stability and maintaining high interfacial kinetics,however,has not yet been resolved.Herein,we design a coherent Li_(1.3)A_(l0.3)Ti_(1.7)(PO)_(4)(LATP)layer that is crystally connected to the spinel LNMO host lattices,which offers fast lithium ions transportation as well as enhances the mechanical stability that prevents the particle fracture.Furthermore,the inactive Li_(3)BO_(3)(LBO)coating layer inhibits the corrosion of transition metals and continuous side reactions.Consequently,the coherent-engineered LNMO-LATPLBO cathode material exhibits superior electrochemical cycling stability in a window of 3.0–5.0 V,for example a high-capacity retention that is 89.7%after 500 cycles at 200 m A g-1obtained and enhanced rate performance(85.1 m A h g^(-1)at 800 m A g^(-1))when tested with a LiPF6-based carbonate electrolyte.Our work presents a new approach of engineering 5 V class spinel oxide cathode that combines interfacial coherent crystal lattice design and surface coating.展开更多
Rechargeable zinc-air batteries(ZABs)are a promising energy conversion device,which rely critically on electrocatalysts to accelerate their rate-determining reactions such as oxygen reduction(ORR)and oxygen evolution ...Rechargeable zinc-air batteries(ZABs)are a promising energy conversion device,which rely critically on electrocatalysts to accelerate their rate-determining reactions such as oxygen reduction(ORR)and oxygen evolution reactions(OER).Herein,we fabricate a range of bifunctional M-N-C(metal-nitrogen-carbon)catalysts containing M-Nx coordination sites and M/MxC nanoparticles(M=Co,Fe,and Cu)using a new class ofγ-cyclodextrin(CD)based metal-organic framework as the precursor.With the two types of active sites interacting with each other in the catalysts,the obtained Fe@C-FeNC and Co@C-CoNC display superior alkaline ORR activity in terms of low half-wave(E1/2)potential(~0.917 and 0.906 V,respectively),which are higher than Cu@C-CuNC(~0.829 V)and the commercial Pt/C(~0.861 V).As a bifunctional electrocatalyst,the Co@C-CoNC exhibits the best performance,showing a bifunctional ORR/OER overpotential(ΔE)of~0.732 V,which is much lower than that of Fe@C-FeNC(~0.831 V)and Cu@C-CuNC(~1.411 V),as well as most of the robust bifunctional electrocatalysts reported to date.Synchrotron X-ray absorption spectroscopy and density functional theory simulations reveal that the strong electronic correlation between metallic Co nanoparticles and the atomic Co-N4 sites in the Co@C-CoNC catalyst can increase the d-electron density near the Fermi level and thus effectively optimize the adsorption/desorption of intermediates in ORR/OER,resulting in an enhanced bifunctional electrocatalytic performance.The Co@C-CoNC-based rechargeable ZAB exhibited a maximum power density of 162.80 mW cm^(−2) at 270.30 mA cm^(−2),higher than the combination of commercial Pt/C+RuO2(~158.90 mW cm^(−2) at 265.80 mA cm^(−2))catalysts.During the galvanostatic discharge at 10 mA cm^(−2),the ZAB delivered an almost stable discharge voltage of 1.2 V for~140 h,signifying the virtue of excellent bifunctional ORR/OER electrocatalytic activity.展开更多
A fuel cell is an energy conversion device that can continuously input fuel and oxidant into the device through an electrochemical reaction to release electrical energy.Although noble metals show good activity in fuel...A fuel cell is an energy conversion device that can continuously input fuel and oxidant into the device through an electrochemical reaction to release electrical energy.Although noble metals show good activity in fuel cell-related electrochemical reactions,their ever-increasing price considerably hinders their industrial application.Improvement of atom utilization efficiency is considered one of the most effective strategies to improve the mass activity of catalysts,and this allows for the use of fewer catalysts,saving greatly on the cost.Thus,single-atom catalysts(SACs)with an atom utilization efficiency of 100%have been widely developed,which show remarkable performance in fuel cells.In this review,we will describe recent progress on the development of SACs for membrane electrode assembly of fuel cell applications.First,we will introduce several effective routes for the synthesis of SACs.The reaction mechanism of the involved reactions will also be introduced as it is highly determinant of the final activity.Then,we will systematically summarize the application of Pt group metal(PGM)and nonprecious group metal(non-PGM)catalysts in membrane electrode assembly of fuel cells.This review will offer numerous experiences for developing potential industrialized fuel cell catalysts in the future.展开更多
MnO_(2)/Melem composites were synthesized with MnO_(2)nanoparticles loaded onto the Melem using the hydrothermal method.As raw materials for C and N carriers,Melem was prepared from melamine roasted at 354℃,and KMnO_...MnO_(2)/Melem composites were synthesized with MnO_(2)nanoparticles loaded onto the Melem using the hydrothermal method.As raw materials for C and N carriers,Melem was prepared from melamine roasted at 354℃,and KMnO_(4)as a raw material for Mn,MnO_(2)nanoparticles were prepared using the hydrothermal synthesis of KMnO_(4).Scanning electron microscopy(SEM),transmission electron microscopy(TEM),X-ray diffraction(XRD),and a laser particle size analyzer were used for structural characterization,and the catalytic oxidation performance of the heavy oil was investigated at different reaction temperatures(100℃to 180℃)using MnO_(2)/Melem with an oxidant and donor protonic acid.The results showed that the synthesizedβ-MnO_(2)nanoparticles were successfully loaded onto the Melem surface;the oil samples before and after the reaction at different temperatures were subjected to SARA analysis using Fourier transform infrared(FT-IR),elemental analysis,gas chromatography-mass spectrometry(GC-MS)and viscosity tests,respectively.It was determined that the hydrocarbons in the crude oil were converted to heavy mass by oxidation reactions with the oxidant mainly through a low-temperature oxidation process below 140℃in the heavy oil when the temperature exceeds 140℃,in addition to the oxidation reaction with the oxidant,a cleavage reaction in the carbon chain occurs to form hydrocarbon substances with lower molecular weights.展开更多
Biomass-derived carbon has demonstrated great potentials as advanced electrode for capacitive deionization(CDI),owing to good electroconductivity,easy availability,intrinsic pores/channels.However,conventional simple ...Biomass-derived carbon has demonstrated great potentials as advanced electrode for capacitive deionization(CDI),owing to good electroconductivity,easy availability,intrinsic pores/channels.However,conventional simple pyrolysis of biomass always generates inadequate porosity with limited surface area.Moreover,biomass-derived carbon also suffers from poor wettability and single physical adsorption of ions,resulting in limited desalination performance.Herein,pore structure optimization and element co-doping are integrated on banana peels(BP)-derived carbon to construct hierarchically porous and B,N co-doped carbon with large ions-accessible surface area.A unique expansionactivation(EA)strategy is proposed to modulate the porosity and specific surface area of carbon.Furthermore,B,N co-doping could increase the ions-accessible sites with improved hydrophilicity,and promote ions adsorption.Benefitting from the synergistic effect of hierarchical porosity and B,N co-doping,the resultant electrode manifest enhanced CDI performance for NaCl with large desalination capacity(29.5 mg g^(-1)),high salt adsorption rate(6.2 mg g^(-1)min^(-1)),and versatile adsorption ability for other salts.Density functional theory reveals the enhanced deionization mechanism by pore and B,N co-doping.This work proposes a facile EA strategy for pore structure modulation of biomass-derived carbon,and demonstrates great potentials of integrating pore and heteroatoms-doping on constructing high-performance CDI electrode.展开更多
The function of solid electrolytes and the composition of solid electrolyte interphase(SEI)are highly significant for inhibiting the growth of Li dendrites.Herein,we report an in-situ interfacial passivation combined ...The function of solid electrolytes and the composition of solid electrolyte interphase(SEI)are highly significant for inhibiting the growth of Li dendrites.Herein,we report an in-situ interfacial passivation combined with self-adaptability strategy to reinforce Li_(0.33)La_(0.557)TiO_(3)(LLTO)-based solid-state batteries.Specifically,a functional SEI enriched with LiF/Li_(3)PO_(4) is formed by in-situ electrochemical conversion,which is greatly beneficial to improving interface compatibility and enhancing ion transport.While the polarized dielectric BaTiO_(3)-polyamic acid(BTO-PAA,BP)film greatly improves the Li-ion transport kinetics and homogenizes the Li deposition.As expected,the resulting electrolyte offers considerable ionic conductivity at room temperature(4.3 x 10~(-4)S cm^(-1))and appreciable electrochemical decomposition voltage(5.23 V)after electrochemical passivation.For Li-LiFePO_(4) batteries,it shows a high specific capacity of 153 mA h g^(-1)at 0.2C after 100 cycles and a long-term durability of 115 mA h g^(-1)at 1.0 C after 800 cycles.Additionally,a stable Li plating/stripping can be achieved for more than 900 h at 0.5 mA cm^(-2).The stabilization mechanisms are elucidated by ex-situ XRD,ex-situ XPS,and ex-situ FTIR techniques,and the corresponding results reveal that the interfacial passivation combined with polarization effect is an effective strategy for improving the electrochemical performance.The present study provides a deeper insight into the dynamic adjustment of electrode-electrolyte interfacial for solid-state lithium batteries.展开更多
Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic properties.However,the high surface energy limits their synthesis,thus creating significant challenges for further de...Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic properties.However,the high surface energy limits their synthesis,thus creating significant challenges for further development.In the last few years,metal–organic frameworks(MOFs)have received significant consideration as ideal candidates for synthesizing SACs due to their tailorable chemistry,tunable morphologies,high porosity,and chemical/thermal stability.From this perspective,this review thoroughly summarizes the previously reported methods and possible future approaches for constructing MOF-based(MOF-derived-supported and MOF-supported)SACs.Then,MOF-based SAC's identification techniques are briefly assessed to understand their coordination environments,local electronic structures,spatial distributions,and catalytic/electrochemical reaction mechanisms.This review systematically highlights several photocatalytic and electrocatalytic applications of MOF-based SACs for energy conversion and storage,including hydrogen evolution reactions,oxygen evolution reactions,O_(2)/CO_(2)/N_(2) reduction reactions,fuel cells,and rechargeable batteries.Some light is also shed on the future development of this highly exciting field by highlighting the advantages and limitations of MOF-based SACs.展开更多
A series of mesoporous phosphotungstic acid/alumina composites(HPW/Al2O3) with various HPW contents were synthesized by evaporation-induced self-assembly method. These composites were characterized by nitrogen adsorpt...A series of mesoporous phosphotungstic acid/alumina composites(HPW/Al2O3) with various HPW contents were synthesized by evaporation-induced self-assembly method. These composites were characterized by nitrogen adsorption-desorption, TEM, FTIR, and UV-vis, and were tested as catalysts in oxidation desulfurization of model fuel composed of dibenzothiophene(DBT) and hydrocarbon, using H2O2as the oxidant. These composites exhibited high activity in catalytic oxidation of DBT in model fuel and good reusing ability. The best performance was achieved by using the mesoporous HPW/Al2O3 with 15wt% HPW content, which resulted in a DBT conversion of 98% after 2 h reaction at 343 K, and it did not show significant activity degradation after 3 recycles. Characterization results showed that the mesoporous structure of alumina and the Keggin structure of HPW were preserved in the formed composite. These results suggested that HPW/Al2O3 could be a promising catalyst in oxidative desulfurization process.展开更多
Mesoporous silica-zirconia supported phosphotungstic acid was synthesized by evaporation induced self-assembly method and used as oxidative desulfurization catalysts. The structural properties of as-prepared catalysts...Mesoporous silica-zirconia supported phosphotungstic acid was synthesized by evaporation induced self-assembly method and used as oxidative desulfurization catalysts. The structural properties of as-prepared catalysts were characterized using various analytical techniques including X-ray diffraction, transmission electron microscopy, Fourier transform infrared spectroscopy, and nitrogen adsorption desorption. The experimental results showed that HPW was highly dispersed on mesoporous framework. The surface acidity of catalysts was analyzed by FTIR measurement of adsorbed pyridine.The surface Lewis acidity was improved with increasing the content of zirconium in the samples. The mesoporous composites were used as catalysts with H2O2 as oxidant for oxidative desulfurization of model fuel. The catalytic activity results showed that the surface Lewis acid sites acted as selective adsorption active sites for dibenzothiophene, which facilitated the sulfur removal from model fuel in the presence of arene. A slight decrease in activity of the recovered catalyst used in the proceeding rounds indicated the reusability of the catalyst.展开更多
Solvothermal reactions of MnCl_2·4H_2O with(pyridin-2-yl)methyl 4-(2-(4-((pyridin-2-yl)methoxy)phenyl)diazenyl)benzoate(L1) via an in situ ligand transformation reaction produced a new coordination polymer, {[Mn_...Solvothermal reactions of MnCl_2·4H_2O with(pyridin-2-yl)methyl 4-(2-(4-((pyridin-2-yl)methoxy)phenyl)diazenyl)benzoate(L1) via an in situ ligand transformation reaction produced a new coordination polymer, {[Mn_(2.5)Cl_3L_2(H_2O)]·H_2O}_n(1, where HL = 4-(2-(4-((pyridin-2-yl)methoxy)phenyl)diazenyl)benzoic acid). The L1 ligand was decomposed in situ to L^- which was coordinated with Mn(Ⅱ) to form compound 1 in the solvothermal synthesis process. Complex 1 was characterized by IR spectroscopy, powder X-ray diffraction and single-crystal X-ray diffraction.Compound 1 possesses a 2D network. In addition, stability and photoluminescent property of 1 were also investigated.展开更多
Nanoparticles of BaLiF3:Er3+ were prepared from the quaternary microemulsions of Cetyltrim-Enthyl Ammonium Bromide (CTAB), n-butanol, n-octane, and water, using the hydrothermal-microemulsion technique. The complex fl...Nanoparticles of BaLiF3:Er3+ were prepared from the quaternary microemulsions of Cetyltrim-Enthyl Ammonium Bromide (CTAB), n-butanol, n-octane, and water, using the hydrothermal-microemulsion technique. The complex fluorides were characterized by means of X-ray power diffraction, Environmental Scanning Electron Microscopy (ESEM), and fluorescence spectra. The positions and in- tensities of the peaks in the XRD pattern of the final products indicate the formation of BaLiF3:Er3+. No other peaks or impurities were de- tected. The average size of the nanoparticles, calculated with the Debye-Scherrer equation was 98.45 nm, which was in agreement with the result of ESEM. The infrared fluorescence spectra consisted of four peaks with a predominant peak located at 1540 nm.展开更多
A novel type of molecular tweezer receptors based on deoxycholic acid has been designed and synthesized and their binding properties were examined by UV-vis spectral titration. These molecular tweezers showed a high s...A novel type of molecular tweezer receptors based on deoxycholic acid has been designed and synthesized and their binding properties were examined by UV-vis spectral titration. These molecular tweezers showed a high selectivity toward F- over Cl-,Br-, I-, AcO-, H2PO4-.展开更多
In this paper,a new method combines chemical/physical crosslinking,and emulsification-foaming porogenic was adopted to prepare n-hydroxyapatite(n-HA)/polyvinyl alcohol(PVA)/chitosan(CS)porous composite hydrogel using ...In this paper,a new method combines chemical/physical crosslinking,and emulsification-foaming porogenic was adopted to prepare n-hydroxyapatite(n-HA)/polyvinyl alcohol(PVA)/chitosan(CS)porous composite hydrogel using artificial cornea scaffold materials.The fabricate conditions,including the type and amount of emulsification-foaming porogen,mixing time and speed etc.were researched.The results showed the optimal condition that the alkylphenol polyoxyethylene ether(OP)acted as emulsification-foaming porogen,with the ratio of WPVA/WOP as 3.75,and mixing 15 min with a stirring speed of 800 r·min-1.Additionally,the fabricated composite hydrogel scaffold materials possessed interconnected internal holes,a moisture content of above 65%,and tensile strength of above 6 MPa.In vitro cytotoxicity and acute systemic toxicity assay confirmed that the scaffolds did not show any cytotoxicity.The as-prepared hydrogel could be a promising candidate for artificial cornea scaffold material.展开更多
[Objective] The aim was to study the brewing technology of apple brandy. [Method] After the activated wine yeast was added to the apple juice by sizing classification, rinsing, falling to pieces and squeezing, the pre...[Objective] The aim was to study the brewing technology of apple brandy. [Method] After the activated wine yeast was added to the apple juice by sizing classification, rinsing, falling to pieces and squeezing, the preceding fermentation began. Every other day, parameters of fermentation broth such as temperature, pH, acidity, sugar content and bubble numbers were detected. Once the sugar content of the fermentation suspension was approaching 5-6 °Bx, the following fermentation would start via pouring wine. After 20-30 days, the cider was changed into original apple brandy by distillation. The last procedure was aging which included man-made speediness aging and oak wood aging about 20 days. The physical and chemical compositions before and after aging were measured. [Result] 22.5 kg apple resulted into 16.56 L of juice. The juice yield was about 73.6% (10 ml/kg). The alcohol rate of distilled apple juice was 20.0%. The color of apple brandy was darker than that of original apple brandy. Alcohol level reduced, but total acidity, fixed acid, lipid and furfural content rose. [Conclusion] The apple brandy was of particular flavor and high quality by selecting befitting fruit, activated wine yeast and feasible brewing, distillation and aging technology. It will be conductive to the development of apple processing industry and the research and development of key brandy technique.展开更多
Two novel coordination polymers with helical chains, {[Zn(L)(H2O)]?H2O}n(1) and {[Zn(L)(p-bix)]?3.5H2O}n(2), where H2 L = 5-(4-hydroxypyridinium-1-ylmethyl) isophthalic acid and p-bix = 1,4-bis(imidazol-1-ylmethyl)ben...Two novel coordination polymers with helical chains, {[Zn(L)(H2O)]?H2O}n(1) and {[Zn(L)(p-bix)]?3.5H2O}n(2), where H2 L = 5-(4-hydroxypyridinium-1-ylmethyl) isophthalic acid and p-bix = 1,4-bis(imidazol-1-ylmethyl)benzene, have been hydrothermally synthesized, and charac-terized by elemental analysis, powder X-ray diffraction(PXRD), IR, thermal gravimetric analyses(TGA) and also by single-crystal X-ray diffraction. Both complexes 1 and 2 crystallize inmonoclinic, space group P21/c. Compound 1 displays a two-dimensional(2D) structure with two distinct types of helical chains; 2 shows a layered coordination polymer with two types of helical chains and features an interesting 2D→3D interdigitated architecture. Meanwhile, the luminescent properties of 1 and 2 have also been investigated in detail.展开更多
A zinc(Ⅱ) coordination polymer [Zn2(2-mBIM)2(SUC)2]n (1, 2-mBIM = bis(2-methylimidazo-1-yl) methane, SUC = succinate anion) has been synthesized and characterized by X-ray diffraction. Complex 1 crystallizes in the t...A zinc(Ⅱ) coordination polymer [Zn2(2-mBIM)2(SUC)2]n (1, 2-mBIM = bis(2-methylimidazo-1-yl) methane, SUC = succinate anion) has been synthesized and characterized by X-ray diffraction. Complex 1 crystallizes in the triclinic space group P1 with a = 9.4871(8), b = 12.9789(5), c = 14.0230(5), α = 90.474(1), β = 90.3560(10), γ = 109.691(1)°, V = 1529.94(15)3 , Z = 2, Dc = 1.553 mg/m3 , μ = 1.63 mm-1 , F(000) = 736, the final R = 0.0645 and wR = 0.0951 for 4067 observed reflections with I > 2σ(I). Each Zn atom was coordinated by two individual 2-mBIM ligands in a cis-conformation and two monodentate coordinated succinate anions in a gauche conformation, resulting in the formation of a two-dimensional supramolecular network containing a cationic 16-membered macrometallacycle and a 28-membered macrometallacycle. The result also indicates that the conformation of the ligands has a strong influence on the structure of the supramolecular network.展开更多
Two new complexes based on 6-hydroxypicolinic acid(H_2picO) and 1,10-phenanthroline(phen), such as [Cu_4(picO)_4(phen)_4]·12 H_2O(1) and {[Cd_4(picO)_4(phen)_4(H_2O)_2]·5H_2O}_n(2), have been synthesized and...Two new complexes based on 6-hydroxypicolinic acid(H_2picO) and 1,10-phenanthroline(phen), such as [Cu_4(picO)_4(phen)_4]·12 H_2O(1) and {[Cd_4(picO)_4(phen)_4(H_2O)_2]·5H_2O}_n(2), have been synthesized and characterized by IR, elemental analyses, thermogravimetric analyses and X-ray diffraction technique. Single-crystal X-ray diffraction analyses revealed that the two complexes both crystallize in the triclinic system, space group P(16)-. For complex 1, the picO ligands adopt a tridentate coordination mode to link copper(Ⅱ) ions into dimmers. PicO ligands also adopt a tridentate mode in complex 2, which connects the cadmium(Ⅱ) to form a one-dimensional chain. Moreover, luminescent properties of 1 and 2 were also investigated.展开更多
Several 1,4-benzenedicarbonyl thiourea resins (BTR) were synthesized through interfacial polymerization between 1,4-benzenedicarbonyl diisothiocyanate and polyamine. Their structures were confirmed by FT-IR. The adsor...Several 1,4-benzenedicarbonyl thiourea resins (BTR) were synthesized through interfacial polymerization between 1,4-benzenedicarbonyl diisothiocyanate and polyamine. Their structures were confirmed by FT-IR. The adsorption properties (including the effect of adsorption time,pH,initial concentrations and temperature) of BTR-1,BTR-2 and BTR-3 for Ag(I) were investigated by batch tests. The results show that the adsorption equilibria of BTR-1,BTR-2,BTR-3 for Ag(I) are achieved after about 10 h. Their equilibrium adsorption capacities are 7.11,6.75 and 6.23,respectively,and the adsorption process accords with G. E. Boyd equation and Langmuir adsorption isotherm as well. The adsorption capacities increase with the increase of pH (the highest uptake values are observed at pH being about 6-7). The thermodynamic parameters of BTR-1 were calculated. The results show that-HΘ and-SΘ are 6 958.8 J/mol and 64.28 J/(mol-K),respectively,and-GΘ at 20,30,40 and 50 °C are-11.79,-12.52,-13.16 and-13.8 kJ/mol,respectively. The silver-loaded resins can be quantitatively eluted by a solution containing 6% thiourea in 1 mol/L HNO3.展开更多
基金supported by the National Natural Science Foundation of China(No.41802179)Sichuan Science and Technology Program(No.2019YFH0037)the Foundation of the State Key Laboratory of Petroleum Resources and Prospecting,China University of Petroleum,Beijing(No.PRP/open-1906).
文摘Recently, significant oil discoveries have been made in the shallower pay zones of the Jurassic Badaowan Formation (J_(1)b) in the Mahu Sag, Junggar Basin, Northwest China. However, little work has been done on the geochemical characteristics and origins of the oil in the J_(1)b reservoir. This study analyzes 44 oil and 14 source rock samples from the area in order to reveal their organic geochemical characteristics and the origins of the oils. The J_(1)b oils are characterized by a low Pr/Ph ratio and high β-carotene and gammacerane indices, which indicate that they were mainly generated from source rocks deposited in a hypersaline environment. The oils are also extremely enhanced in C_(29) regular steranes, possibly derived from halophilic algae. Oil-source correlation shows that the oils were derived from the Lower Permian Fengcheng Formation (P_(1)f) source rocks, which were deposited in a strongly stratified and highly saline water column with a predominance of algal/bacterial input in the organic matter. The source rocks of the Middle Permian lower-Wuerhe Formation (P_(2)w), which were deposited in fresh to slightly saline water conditions with a greater input of terrigenous organic matter, make only a minor contribution to the J_(1)b oils. The reconstruction of the oil accumulation process shows that the J_(1)b oil reservoir may have been twice charged during Late Jurassic–Early Cretaceous and the Paleogene–Neogene, respectively. A large amount volume of hydrocarbons generated in the P_(1)f source rock and leaked from T_(1)b oil reservoirs migrated along faults connecting source beds and shallow-buried secondary faults into Jurassic traps, resulting in large-scale accumulations in J_(1)b. These results are crucial for understanding the petroleum system of the Mahu Sag and will provide valuable guidance for petroleum exploration in the shallower formations in the slope area of the sag.
基金supported by the Natural Science Foundation of Jiangsu Province(BK20200800)the National Natural Science Foundation of China(22209075,51902165,12004145)+1 种基金the Natural Science Foundation of Jiangxi Province(20212BAB214032,20192ACBL20048)the Key Science and Technology Plan Project of Ji’an City(20211-015311)。
文摘Spinel LiNi_(0.5)Mn_(1.5)O_(4)(LNMO),a 5 V class high voltage cathode,has been regarded as an attractive candidate to further improve the energy density of lithium-ion battery.The issue simultaneously enabling side stability and maintaining high interfacial kinetics,however,has not yet been resolved.Herein,we design a coherent Li_(1.3)A_(l0.3)Ti_(1.7)(PO)_(4)(LATP)layer that is crystally connected to the spinel LNMO host lattices,which offers fast lithium ions transportation as well as enhances the mechanical stability that prevents the particle fracture.Furthermore,the inactive Li_(3)BO_(3)(LBO)coating layer inhibits the corrosion of transition metals and continuous side reactions.Consequently,the coherent-engineered LNMO-LATPLBO cathode material exhibits superior electrochemical cycling stability in a window of 3.0–5.0 V,for example a high-capacity retention that is 89.7%after 500 cycles at 200 m A g-1obtained and enhanced rate performance(85.1 m A h g^(-1)at 800 m A g^(-1))when tested with a LiPF6-based carbonate electrolyte.Our work presents a new approach of engineering 5 V class spinel oxide cathode that combines interfacial coherent crystal lattice design and surface coating.
基金supported by the Shenzhen Government’s Plan of Science and Technology(JCYJ20190808121407676 and 20200813142301001)National Natural Science Foundation of China(22178223 and 22262010)+1 种基金Guangxi Science and Technology Fund for Distinguished High-Talent Introduction Program(No.RZ2200002233AC22035091).
文摘Rechargeable zinc-air batteries(ZABs)are a promising energy conversion device,which rely critically on electrocatalysts to accelerate their rate-determining reactions such as oxygen reduction(ORR)and oxygen evolution reactions(OER).Herein,we fabricate a range of bifunctional M-N-C(metal-nitrogen-carbon)catalysts containing M-Nx coordination sites and M/MxC nanoparticles(M=Co,Fe,and Cu)using a new class ofγ-cyclodextrin(CD)based metal-organic framework as the precursor.With the two types of active sites interacting with each other in the catalysts,the obtained Fe@C-FeNC and Co@C-CoNC display superior alkaline ORR activity in terms of low half-wave(E1/2)potential(~0.917 and 0.906 V,respectively),which are higher than Cu@C-CuNC(~0.829 V)and the commercial Pt/C(~0.861 V).As a bifunctional electrocatalyst,the Co@C-CoNC exhibits the best performance,showing a bifunctional ORR/OER overpotential(ΔE)of~0.732 V,which is much lower than that of Fe@C-FeNC(~0.831 V)and Cu@C-CuNC(~1.411 V),as well as most of the robust bifunctional electrocatalysts reported to date.Synchrotron X-ray absorption spectroscopy and density functional theory simulations reveal that the strong electronic correlation between metallic Co nanoparticles and the atomic Co-N4 sites in the Co@C-CoNC catalyst can increase the d-electron density near the Fermi level and thus effectively optimize the adsorption/desorption of intermediates in ORR/OER,resulting in an enhanced bifunctional electrocatalytic performance.The Co@C-CoNC-based rechargeable ZAB exhibited a maximum power density of 162.80 mW cm^(−2) at 270.30 mA cm^(−2),higher than the combination of commercial Pt/C+RuO2(~158.90 mW cm^(−2) at 265.80 mA cm^(−2))catalysts.During the galvanostatic discharge at 10 mA cm^(−2),the ZAB delivered an almost stable discharge voltage of 1.2 V for~140 h,signifying the virtue of excellent bifunctional ORR/OER electrocatalytic activity.
基金National Natural Science Foundation of China,Grant/Award Numbers:22075203,22279079,21905179Guangdong Science and Technology Department Program,Grant/Award Number:2021QN02L252+1 种基金Shenzhen Science and Technology Department Program,Grant/Award Numbers:20220810133521001,20220809165014001Natural Science Foundation of SZU,Grant/Award Numbers:000002111605,000002112215。
文摘A fuel cell is an energy conversion device that can continuously input fuel and oxidant into the device through an electrochemical reaction to release electrical energy.Although noble metals show good activity in fuel cell-related electrochemical reactions,their ever-increasing price considerably hinders their industrial application.Improvement of atom utilization efficiency is considered one of the most effective strategies to improve the mass activity of catalysts,and this allows for the use of fewer catalysts,saving greatly on the cost.Thus,single-atom catalysts(SACs)with an atom utilization efficiency of 100%have been widely developed,which show remarkable performance in fuel cells.In this review,we will describe recent progress on the development of SACs for membrane electrode assembly of fuel cell applications.First,we will introduce several effective routes for the synthesis of SACs.The reaction mechanism of the involved reactions will also be introduced as it is highly determinant of the final activity.Then,we will systematically summarize the application of Pt group metal(PGM)and nonprecious group metal(non-PGM)catalysts in membrane electrode assembly of fuel cells.This review will offer numerous experiences for developing potential industrialized fuel cell catalysts in the future.
基金supported by the National Natural Science Foundation of China (51472034)the Key Laboratory Development Fund of Hubei Province (202305904)the Cooperation Project of Petro China Tahe Oilfield Company (2021H10005)。
文摘MnO_(2)/Melem composites were synthesized with MnO_(2)nanoparticles loaded onto the Melem using the hydrothermal method.As raw materials for C and N carriers,Melem was prepared from melamine roasted at 354℃,and KMnO_(4)as a raw material for Mn,MnO_(2)nanoparticles were prepared using the hydrothermal synthesis of KMnO_(4).Scanning electron microscopy(SEM),transmission electron microscopy(TEM),X-ray diffraction(XRD),and a laser particle size analyzer were used for structural characterization,and the catalytic oxidation performance of the heavy oil was investigated at different reaction temperatures(100℃to 180℃)using MnO_(2)/Melem with an oxidant and donor protonic acid.The results showed that the synthesizedβ-MnO_(2)nanoparticles were successfully loaded onto the Melem surface;the oil samples before and after the reaction at different temperatures were subjected to SARA analysis using Fourier transform infrared(FT-IR),elemental analysis,gas chromatography-mass spectrometry(GC-MS)and viscosity tests,respectively.It was determined that the hydrocarbons in the crude oil were converted to heavy mass by oxidation reactions with the oxidant mainly through a low-temperature oxidation process below 140℃in the heavy oil when the temperature exceeds 140℃,in addition to the oxidation reaction with the oxidant,a cleavage reaction in the carbon chain occurs to form hydrocarbon substances with lower molecular weights.
基金We gratefully acknowledge financial supports from the National Natural Science Foundation of China(No.52202371,51905125,52102364)the Natural Science Foundation of Shandong Province(No.ZR2020QE066)+2 种基金Opening Project of State Key Laboratory of Advanced Technology for Float Glass(No.2020KF08)SDUT&Zibo City Integration Development Project(No.2021SNPT0045)the fellowship of China Postdoctoral Science Foundation(No.2020M672081).
文摘Biomass-derived carbon has demonstrated great potentials as advanced electrode for capacitive deionization(CDI),owing to good electroconductivity,easy availability,intrinsic pores/channels.However,conventional simple pyrolysis of biomass always generates inadequate porosity with limited surface area.Moreover,biomass-derived carbon also suffers from poor wettability and single physical adsorption of ions,resulting in limited desalination performance.Herein,pore structure optimization and element co-doping are integrated on banana peels(BP)-derived carbon to construct hierarchically porous and B,N co-doped carbon with large ions-accessible surface area.A unique expansionactivation(EA)strategy is proposed to modulate the porosity and specific surface area of carbon.Furthermore,B,N co-doping could increase the ions-accessible sites with improved hydrophilicity,and promote ions adsorption.Benefitting from the synergistic effect of hierarchical porosity and B,N co-doping,the resultant electrode manifest enhanced CDI performance for NaCl with large desalination capacity(29.5 mg g^(-1)),high salt adsorption rate(6.2 mg g^(-1)min^(-1)),and versatile adsorption ability for other salts.Density functional theory reveals the enhanced deionization mechanism by pore and B,N co-doping.This work proposes a facile EA strategy for pore structure modulation of biomass-derived carbon,and demonstrates great potentials of integrating pore and heteroatoms-doping on constructing high-performance CDI electrode.
基金financially supported by the National Natural Science Foundation of China (51971080)the Shenzhen Bureau of Science,Technology and Innovation Commission (GXWD20201230155427003-20200730151200003 and JSGG20200914113601003)。
文摘The function of solid electrolytes and the composition of solid electrolyte interphase(SEI)are highly significant for inhibiting the growth of Li dendrites.Herein,we report an in-situ interfacial passivation combined with self-adaptability strategy to reinforce Li_(0.33)La_(0.557)TiO_(3)(LLTO)-based solid-state batteries.Specifically,a functional SEI enriched with LiF/Li_(3)PO_(4) is formed by in-situ electrochemical conversion,which is greatly beneficial to improving interface compatibility and enhancing ion transport.While the polarized dielectric BaTiO_(3)-polyamic acid(BTO-PAA,BP)film greatly improves the Li-ion transport kinetics and homogenizes the Li deposition.As expected,the resulting electrolyte offers considerable ionic conductivity at room temperature(4.3 x 10~(-4)S cm^(-1))and appreciable electrochemical decomposition voltage(5.23 V)after electrochemical passivation.For Li-LiFePO_(4) batteries,it shows a high specific capacity of 153 mA h g^(-1)at 0.2C after 100 cycles and a long-term durability of 115 mA h g^(-1)at 1.0 C after 800 cycles.Additionally,a stable Li plating/stripping can be achieved for more than 900 h at 0.5 mA cm^(-2).The stabilization mechanisms are elucidated by ex-situ XRD,ex-situ XPS,and ex-situ FTIR techniques,and the corresponding results reveal that the interfacial passivation combined with polarization effect is an effective strategy for improving the electrochemical performance.The present study provides a deeper insight into the dynamic adjustment of electrode-electrolyte interfacial for solid-state lithium batteries.
基金support from the Shenzhen Science and Technology Program(No.KQTD20190929173914967,ZDSYS20220527171401003,and JCYJ20200109110416441).
文摘Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic properties.However,the high surface energy limits their synthesis,thus creating significant challenges for further development.In the last few years,metal–organic frameworks(MOFs)have received significant consideration as ideal candidates for synthesizing SACs due to their tailorable chemistry,tunable morphologies,high porosity,and chemical/thermal stability.From this perspective,this review thoroughly summarizes the previously reported methods and possible future approaches for constructing MOF-based(MOF-derived-supported and MOF-supported)SACs.Then,MOF-based SAC's identification techniques are briefly assessed to understand their coordination environments,local electronic structures,spatial distributions,and catalytic/electrochemical reaction mechanisms.This review systematically highlights several photocatalytic and electrocatalytic applications of MOF-based SACs for energy conversion and storage,including hydrogen evolution reactions,oxygen evolution reactions,O_(2)/CO_(2)/N_(2) reduction reactions,fuel cells,and rechargeable batteries.Some light is also shed on the future development of this highly exciting field by highlighting the advantages and limitations of MOF-based SACs.
基金Funded by the National Natural Science Foundation of China(21106008)the PetroChina Innovation Foundation(2013D-5006-0405)the Natural Science Foundation of Hubei Province(2011CDB007)
文摘A series of mesoporous phosphotungstic acid/alumina composites(HPW/Al2O3) with various HPW contents were synthesized by evaporation-induced self-assembly method. These composites were characterized by nitrogen adsorption-desorption, TEM, FTIR, and UV-vis, and were tested as catalysts in oxidation desulfurization of model fuel composed of dibenzothiophene(DBT) and hydrocarbon, using H2O2as the oxidant. These composites exhibited high activity in catalytic oxidation of DBT in model fuel and good reusing ability. The best performance was achieved by using the mesoporous HPW/Al2O3 with 15wt% HPW content, which resulted in a DBT conversion of 98% after 2 h reaction at 343 K, and it did not show significant activity degradation after 3 recycles. Characterization results showed that the mesoporous structure of alumina and the Keggin structure of HPW were preserved in the formed composite. These results suggested that HPW/Al2O3 could be a promising catalyst in oxidative desulfurization process.
基金Funded by the National Natural Science Foundation of China(No.21106008)the Petro China Innovation Foundation(No.2013D-5006-0405)
文摘Mesoporous silica-zirconia supported phosphotungstic acid was synthesized by evaporation induced self-assembly method and used as oxidative desulfurization catalysts. The structural properties of as-prepared catalysts were characterized using various analytical techniques including X-ray diffraction, transmission electron microscopy, Fourier transform infrared spectroscopy, and nitrogen adsorption desorption. The experimental results showed that HPW was highly dispersed on mesoporous framework. The surface acidity of catalysts was analyzed by FTIR measurement of adsorbed pyridine.The surface Lewis acidity was improved with increasing the content of zirconium in the samples. The mesoporous composites were used as catalysts with H2O2 as oxidant for oxidative desulfurization of model fuel. The catalytic activity results showed that the surface Lewis acid sites acted as selective adsorption active sites for dibenzothiophene, which facilitated the sulfur removal from model fuel in the presence of arene. A slight decrease in activity of the recovered catalyst used in the proceeding rounds indicated the reusability of the catalyst.
基金financially supported by the National Natural Science Foundation of China(21302003)the Science and Technology Project of Henan Province(No.182102210200)
文摘Solvothermal reactions of MnCl_2·4H_2O with(pyridin-2-yl)methyl 4-(2-(4-((pyridin-2-yl)methoxy)phenyl)diazenyl)benzoate(L1) via an in situ ligand transformation reaction produced a new coordination polymer, {[Mn_(2.5)Cl_3L_2(H_2O)]·H_2O}_n(1, where HL = 4-(2-(4-((pyridin-2-yl)methoxy)phenyl)diazenyl)benzoic acid). The L1 ligand was decomposed in situ to L^- which was coordinated with Mn(Ⅱ) to form compound 1 in the solvothermal synthesis process. Complex 1 was characterized by IR spectroscopy, powder X-ray diffraction and single-crystal X-ray diffraction.Compound 1 possesses a 2D network. In addition, stability and photoluminescent property of 1 were also investigated.
基金Project supported by the Foundation of Science and Technology Department of Jilin Province (20050507)
文摘Nanoparticles of BaLiF3:Er3+ were prepared from the quaternary microemulsions of Cetyltrim-Enthyl Ammonium Bromide (CTAB), n-butanol, n-octane, and water, using the hydrothermal-microemulsion technique. The complex fluorides were characterized by means of X-ray power diffraction, Environmental Scanning Electron Microscopy (ESEM), and fluorescence spectra. The positions and in- tensities of the peaks in the XRD pattern of the final products indicate the formation of BaLiF3:Er3+. No other peaks or impurities were de- tected. The average size of the nanoparticles, calculated with the Debye-Scherrer equation was 98.45 nm, which was in agreement with the result of ESEM. The infrared fluorescence spectra consisted of four peaks with a predominant peak located at 1540 nm.
基金We are very grateful to the National Natural Science Foundation of China(No.20272038)for the financial support.
文摘A novel type of molecular tweezer receptors based on deoxycholic acid has been designed and synthesized and their binding properties were examined by UV-vis spectral titration. These molecular tweezers showed a high selectivity toward F- over Cl-,Br-, I-, AcO-, H2PO4-.
基金Supported by the Key Technology R&D Program of Shenzhen Municipal(JSGG20120614164013545)Basic Research Program of Shenzhen Municipal(JCYJ20130329102614715).
文摘In this paper,a new method combines chemical/physical crosslinking,and emulsification-foaming porogenic was adopted to prepare n-hydroxyapatite(n-HA)/polyvinyl alcohol(PVA)/chitosan(CS)porous composite hydrogel using artificial cornea scaffold materials.The fabricate conditions,including the type and amount of emulsification-foaming porogen,mixing time and speed etc.were researched.The results showed the optimal condition that the alkylphenol polyoxyethylene ether(OP)acted as emulsification-foaming porogen,with the ratio of WPVA/WOP as 3.75,and mixing 15 min with a stirring speed of 800 r·min-1.Additionally,the fabricated composite hydrogel scaffold materials possessed interconnected internal holes,a moisture content of above 65%,and tensile strength of above 6 MPa.In vitro cytotoxicity and acute systemic toxicity assay confirmed that the scaffolds did not show any cytotoxicity.The as-prepared hydrogel could be a promising candidate for artificial cornea scaffold material.
文摘[Objective] The aim was to study the brewing technology of apple brandy. [Method] After the activated wine yeast was added to the apple juice by sizing classification, rinsing, falling to pieces and squeezing, the preceding fermentation began. Every other day, parameters of fermentation broth such as temperature, pH, acidity, sugar content and bubble numbers were detected. Once the sugar content of the fermentation suspension was approaching 5-6 °Bx, the following fermentation would start via pouring wine. After 20-30 days, the cider was changed into original apple brandy by distillation. The last procedure was aging which included man-made speediness aging and oak wood aging about 20 days. The physical and chemical compositions before and after aging were measured. [Result] 22.5 kg apple resulted into 16.56 L of juice. The juice yield was about 73.6% (10 ml/kg). The alcohol rate of distilled apple juice was 20.0%. The color of apple brandy was darker than that of original apple brandy. Alcohol level reduced, but total acidity, fixed acid, lipid and furfural content rose. [Conclusion] The apple brandy was of particular flavor and high quality by selecting befitting fruit, activated wine yeast and feasible brewing, distillation and aging technology. It will be conductive to the development of apple processing industry and the research and development of key brandy technique.
基金supported by Education Chamber of Henan Province(No.15A150068)
文摘Two novel coordination polymers with helical chains, {[Zn(L)(H2O)]?H2O}n(1) and {[Zn(L)(p-bix)]?3.5H2O}n(2), where H2 L = 5-(4-hydroxypyridinium-1-ylmethyl) isophthalic acid and p-bix = 1,4-bis(imidazol-1-ylmethyl)benzene, have been hydrothermally synthesized, and charac-terized by elemental analysis, powder X-ray diffraction(PXRD), IR, thermal gravimetric analyses(TGA) and also by single-crystal X-ray diffraction. Both complexes 1 and 2 crystallize inmonoclinic, space group P21/c. Compound 1 displays a two-dimensional(2D) structure with two distinct types of helical chains; 2 shows a layered coordination polymer with two types of helical chains and features an interesting 2D→3D interdigitated architecture. Meanwhile, the luminescent properties of 1 and 2 have also been investigated in detail.
基金supported by the National Natural Science Foundation of China (No. 21171053)the Science Foundation of HBDE (Z20102501)the Open Research Foundation in the State Key Laboratory of Coordination Chemistry
文摘A zinc(Ⅱ) coordination polymer [Zn2(2-mBIM)2(SUC)2]n (1, 2-mBIM = bis(2-methylimidazo-1-yl) methane, SUC = succinate anion) has been synthesized and characterized by X-ray diffraction. Complex 1 crystallizes in the triclinic space group P1 with a = 9.4871(8), b = 12.9789(5), c = 14.0230(5), α = 90.474(1), β = 90.3560(10), γ = 109.691(1)°, V = 1529.94(15)3 , Z = 2, Dc = 1.553 mg/m3 , μ = 1.63 mm-1 , F(000) = 736, the final R = 0.0645 and wR = 0.0951 for 4067 observed reflections with I > 2σ(I). Each Zn atom was coordinated by two individual 2-mBIM ligands in a cis-conformation and two monodentate coordinated succinate anions in a gauche conformation, resulting in the formation of a two-dimensional supramolecular network containing a cationic 16-membered macrometallacycle and a 28-membered macrometallacycle. The result also indicates that the conformation of the ligands has a strong influence on the structure of the supramolecular network.
基金financially supported by the National Natural Science Foundation of China(21302003)the Science and Technology Project of Henan Province(No.182102210200)
文摘Two new complexes based on 6-hydroxypicolinic acid(H_2picO) and 1,10-phenanthroline(phen), such as [Cu_4(picO)_4(phen)_4]·12 H_2O(1) and {[Cd_4(picO)_4(phen)_4(H_2O)_2]·5H_2O}_n(2), have been synthesized and characterized by IR, elemental analyses, thermogravimetric analyses and X-ray diffraction technique. Single-crystal X-ray diffraction analyses revealed that the two complexes both crystallize in the triclinic system, space group P(16)-. For complex 1, the picO ligands adopt a tridentate coordination mode to link copper(Ⅱ) ions into dimmers. PicO ligands also adopt a tridentate mode in complex 2, which connects the cadmium(Ⅱ) to form a one-dimensional chain. Moreover, luminescent properties of 1 and 2 were also investigated.
基金Projects(20476105, 50604016) supported by the National Natural Science Foundation of China
文摘Several 1,4-benzenedicarbonyl thiourea resins (BTR) were synthesized through interfacial polymerization between 1,4-benzenedicarbonyl diisothiocyanate and polyamine. Their structures were confirmed by FT-IR. The adsorption properties (including the effect of adsorption time,pH,initial concentrations and temperature) of BTR-1,BTR-2 and BTR-3 for Ag(I) were investigated by batch tests. The results show that the adsorption equilibria of BTR-1,BTR-2,BTR-3 for Ag(I) are achieved after about 10 h. Their equilibrium adsorption capacities are 7.11,6.75 and 6.23,respectively,and the adsorption process accords with G. E. Boyd equation and Langmuir adsorption isotherm as well. The adsorption capacities increase with the increase of pH (the highest uptake values are observed at pH being about 6-7). The thermodynamic parameters of BTR-1 were calculated. The results show that-HΘ and-SΘ are 6 958.8 J/mol and 64.28 J/(mol-K),respectively,and-GΘ at 20,30,40 and 50 °C are-11.79,-12.52,-13.16 and-13.8 kJ/mol,respectively. The silver-loaded resins can be quantitatively eluted by a solution containing 6% thiourea in 1 mol/L HNO3.
