Recently, the surface chemical functionalization and morphology control of precious metal nanostructures have been recognized as two efficient strategies for improving their electroactivity and/or selectivity. In this...Recently, the surface chemical functionalization and morphology control of precious metal nanostructures have been recognized as two efficient strategies for improving their electroactivity and/or selectivity. In this work, 1, 10-phenanthroline monohydrate(PM) functionalized Pt nanodendrites(Pt-NDs) on carbon cloth(CC)(denoted as PM@Pt-NDs/CC) and polyethylenimine(PEI) functionalized Pt-NDs on CC(denoted as PEI@Pt-NDs/CC) are successfully achieved by immersing Pt-NDs/CC into PM and PEI aqueous solutions, respectively. PEI functionalization of Pt-NDs/CC improves its electroactivity for hydrogen evolution reaction(HER) due to local proton enrichment whereas PM functionalization of Pt-NDs/CC improves its electroactivity for formic acid oxidation reaction(FAOR) by facilitating dehydrogenation pathway. With such high activity, a two-electrode electrolyzer is assembled using PM@Pt-NDs/CC as the anodic electrocatalyst and PEI@Pt-NDs/CC as the cathodic electrocatalyst for electrochemical reforming of formic acid, which only requires 0.45 V voltage to achieve the current density of 10 mA cm^(-1) for highpurity hydrogen production, much lower than conventional water electrolysis(1.59 V). The work presents an example of interfacial engineering enhancing electrocatalytic activity and indicates that electrochemical reforming of formic acid is an energy-saving electrochemical method for high-purity hydrogen production.展开更多
With the efforts of scientists around the world,the power conversion efficiency(PCE)of perovskite solar cells(PSCs)has reached 25.7%.To further improve the efficiency and break through the Shockley-Queisser(S-Q)limit,...With the efforts of scientists around the world,the power conversion efficiency(PCE)of perovskite solar cells(PSCs)has reached 25.7%.To further improve the efficiency and break through the Shockley-Queisser(S-Q)limit,it is promising to construct all-perovskite tandem solar cells via combining wide-bandgap and narrow-bandgap perovskites[1−5].As the key light-harvesting material for the bottom cell in all-per-ovskite tandem devices,the narrow-bandgap Pb-Sn mixed per-ovskites have attracted increasing interest in recent years[6−8].However,the Pb-Sn mixed perovskites suffer from uncontrol-lable crystallization,easy oxidation of Sn2+and high defect density,which significantly limit PCE improvement[9,10].Organ-ic ammonium halides can improve the efficiency and stabil-ity of Pb-Sn mixed PSCs.展开更多
Inefficient electrocatalysts and high-power consumption are two thorny problems for electrochemical hydrogen(H2)production from acidic water electrolysis.Herein we report the one-pot precise synthesis of ultrafine Au ...Inefficient electrocatalysts and high-power consumption are two thorny problems for electrochemical hydrogen(H2)production from acidic water electrolysis.Herein we report the one-pot precise synthesis of ultrafine Au core-Pt Au alloy shell nanowires(Au@PtxAu UFNWs).Among them,Au@Pt_(0.077) Au UFNWs exhibit the best performance for formic acid oxidation reaction(FAOR)and hydrogen evolution reaction(HER),which only require applied potentials of 0.29 V and-22.6 m V to achieve a current density of 10 m A cm^(-2),respectively.The corresponding formic acid electrolyzer realizes the electrochemical H2 production at a voltage of only 0.51 V with 10 m A cm^(-2) current density.Density functional theory(DFT)calculations reveal that the Au-riched Pt Au alloy structure can facilitates the direct oxidation pathway of FAOR and consequently elevates the FAOR activity of Au@Pt_(0.077) Au UFNWs.This work provides meaningful insights into the electrochemical H_(2) production from both the construction of advanced bifunctional electrocatalysts and the replacement of OER.展开更多
Approach to highly efficient dye-sensitized solar cells(DSSCs)by co-sensitization of organic dyes,AZ6+AZ5 with co-adsorbent chenodeoxycholic acid(CDCA)is presented.The power conversion efficiencies(PCEs)of 8.55%and 8....Approach to highly efficient dye-sensitized solar cells(DSSCs)by co-sensitization of organic dyes,AZ6+AZ5 with co-adsorbent chenodeoxycholic acid(CDCA)is presented.The power conversion efficiencies(PCEs)of 8.55%and 8.31%are obtained from DSSCs co-sensitized by AZ6(0.3 mmol/L)+AZ5(0.1 mmol/L)with CDCA concentration of 5 and 20 mmol/L in one step cocktail,respectively.The latter shows high stability in a period of 653 h under ambient conditions.展开更多
Perovskite solar cell(PSC) is now a shining star in photovoltaics field[1].Benefiting from excellent optoelectronic properties of perovskite materials,the certified power conversion efficiency(PCE)of PSCs has reached ...Perovskite solar cell(PSC) is now a shining star in photovoltaics field[1].Benefiting from excellent optoelectronic properties of perovskite materials,the certified power conversion efficiency(PCE)of PSCs has reached 26.0%[2],showing great potential for commercialization.In essence,the efficiency of solar cells is determined by the radiative and nonradiative recombination of photogenerated charge carriers.The unfavorable nonradiative recombination mainly assisted by the trap states leads to severe charge carrier loss and thus unsatisfactory efficiency.展开更多
Highly effident metal-free, carbon-based, bi-functional electrocatalysts for the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) have attracted increased attention for use in electrochemical en...Highly effident metal-free, carbon-based, bi-functional electrocatalysts for the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) have attracted increased attention for use in electrochemical energy conversion systems, owing to their low cost and high activity. In this work, N-doped carbon nanocages (N-CCs) with a porous self-supported architecture and high specific surface area are synthesized by a facile interfacial assembly synthetic route. The materials are comprehensively characterized by scanning electron microscop36 transmission electron microscopy, nitrogen adsorption-desorption experiments, X-ray diffraction, and X-ray photoelectron spectroscopy. Cyclic voltammetry , chronoamperometry, and linear sweep voltammetry demonstrate that the as-prepared N-CC could serve as an effective metal-free electrocatalyst with excellent catalytic activity, long-term operation durability, and excellent methanol tolerance for the ORR in alkaline media. In the presence of 3 mM methanol, the half wave potential of the N-CCs for the ORR is 190 mV; this is more positive than that of the commercial Pt/C electrocatalyst. Meanwhile, the N-CCs also show an OER activity comparable to that of the commercial Ru/C electrocatalyst, revealing their bifunctional property.展开更多
Catalysts for the oxygen reduction reaction (ORR) play an important role in fuel cells. Alternative non-precious metal catalysts with comparable ORR activity to Pt-based catalysts are highly desirable for the develo...Catalysts for the oxygen reduction reaction (ORR) play an important role in fuel cells. Alternative non-precious metal catalysts with comparable ORR activity to Pt-based catalysts are highly desirable for the development of fuel cells. In this work, we report for the first time a spinel MnC0204/C ORR catalyst consisting of uniform MnC0204 nanoparticles cross-linked with two-dimensional (2D) porous carbon nanosheets (abbreviated as porous MnC0204/C nanosheets), in which glucose is used as the carbon source and NaC1 as the template. The obtained porous MnCo204/C nanosheets present the combined properties of an interconnected porous architecture and a large surface area (175.3 m2-g-1), as well as good electrical conductivity (1.15 x 102 S.cm-1). Thus, the as-prepared MnC0204/C nanosheets efficiently facilitate electrolyte diffusion and offer an expedite transport path for reactants and electrons during the ORR. As a result, the as-prepared porous MnC0204/C nanosheet catalyst exhibits enhanced ORR activity with a higher onset potential and current density than those of its counterparts, including pure MnC0204, carbon nanosheets, and Vulcan XC-72R carbon. More importantly, the porous MnC0204/C nanosheets exhibit a com- parable electrocatalytic activity but superior stability and tolerance toward methanol crossover effects than a high-performance Pt/C catalyst in alkaline medium. The synthetic strategy outlined here can be extended to other non- precious metal catalysts for application in electrochemical energy conversion.展开更多
基金sponsored by Natural Science Foundation of Shaanxi Province (2020JZ-23)the Fundamental Research Funds for the Central Universities (GK201901002, GK201701007 and GK201902014)the 111 Project (B14041)。
文摘Recently, the surface chemical functionalization and morphology control of precious metal nanostructures have been recognized as two efficient strategies for improving their electroactivity and/or selectivity. In this work, 1, 10-phenanthroline monohydrate(PM) functionalized Pt nanodendrites(Pt-NDs) on carbon cloth(CC)(denoted as PM@Pt-NDs/CC) and polyethylenimine(PEI) functionalized Pt-NDs on CC(denoted as PEI@Pt-NDs/CC) are successfully achieved by immersing Pt-NDs/CC into PM and PEI aqueous solutions, respectively. PEI functionalization of Pt-NDs/CC improves its electroactivity for hydrogen evolution reaction(HER) due to local proton enrichment whereas PM functionalization of Pt-NDs/CC improves its electroactivity for formic acid oxidation reaction(FAOR) by facilitating dehydrogenation pathway. With such high activity, a two-electrode electrolyzer is assembled using PM@Pt-NDs/CC as the anodic electrocatalyst and PEI@Pt-NDs/CC as the cathodic electrocatalyst for electrochemical reforming of formic acid, which only requires 0.45 V voltage to achieve the current density of 10 mA cm^(-1) for highpurity hydrogen production, much lower than conventional water electrolysis(1.59 V). The work presents an example of interfacial engineering enhancing electrocatalytic activity and indicates that electrochemical reforming of formic acid is an energy-saving electrochemical method for high-purity hydrogen production.
基金the 111 Project(B21005)the National Natural Science Foundation of China(62174103)+2 种基金the Fundamental Research Funds for the Central Universities(GK202103108)fund of Songshan Lake Materials Laboratory(2021SLABFK02)the National Natural Science Foundation of China(21961160720).
文摘With the efforts of scientists around the world,the power conversion efficiency(PCE)of perovskite solar cells(PSCs)has reached 25.7%.To further improve the efficiency and break through the Shockley-Queisser(S-Q)limit,it is promising to construct all-perovskite tandem solar cells via combining wide-bandgap and narrow-bandgap perovskites[1−5].As the key light-harvesting material for the bottom cell in all-per-ovskite tandem devices,the narrow-bandgap Pb-Sn mixed per-ovskites have attracted increasing interest in recent years[6−8].However,the Pb-Sn mixed perovskites suffer from uncontrol-lable crystallization,easy oxidation of Sn2+and high defect density,which significantly limit PCE improvement[9,10].Organ-ic ammonium halides can improve the efficiency and stabil-ity of Pb-Sn mixed PSCs.
基金supported by the Natural Science Foundation of Shaanxi Province(2020JZ-23)the Fundamental Research Funds for the Central Universities(GK201901002,GK202101005,2020CSLZ012 and 2019TS007)+4 种基金the Innovation Team Project for Graduate Student at Shaanxi Normal University(TD2020048Y)the Key Research and Development Program of Shaanxi(Program No.2020SF-355)the National Training Program of Innovation and Entrepreneurship for Undergraduates(S202010718130)the Open Foundation of Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials at Guangxi University(2021GXYSOF02)the 111 Project(B14041)。
文摘Inefficient electrocatalysts and high-power consumption are two thorny problems for electrochemical hydrogen(H2)production from acidic water electrolysis.Herein we report the one-pot precise synthesis of ultrafine Au core-Pt Au alloy shell nanowires(Au@PtxAu UFNWs).Among them,Au@Pt_(0.077) Au UFNWs exhibit the best performance for formic acid oxidation reaction(FAOR)and hydrogen evolution reaction(HER),which only require applied potentials of 0.29 V and-22.6 m V to achieve a current density of 10 m A cm^(-2),respectively.The corresponding formic acid electrolyzer realizes the electrochemical H2 production at a voltage of only 0.51 V with 10 m A cm^(-2) current density.Density functional theory(DFT)calculations reveal that the Au-riched Pt Au alloy structure can facilitates the direct oxidation pathway of FAOR and consequently elevates the FAOR activity of Au@Pt_(0.077) Au UFNWs.This work provides meaningful insights into the electrochemical H_(2) production from both the construction of advanced bifunctional electrocatalysts and the replacement of OER.
基金Research was supported by the Changjiang Scholars and Innovative Research Team in University(No.IRT1070)the Natural Science Foundation of China(No.51373092)+2 种基金the Specialized Research Fund for the Doc-toral Program of Higher Education of China(No.20130202120010)the Key Science and Technology Program of Shaanxi Province,China(No.2012K08-09)the State Education Ministry and the Fundamental Re-search Funds for the Central Universities(Nos.GK201302036,GK201302037).Our special thanks are also for the Fund of New Energy Devices and Materials provided by Mr.He Chong Ben,Hong Kong.
文摘Approach to highly efficient dye-sensitized solar cells(DSSCs)by co-sensitization of organic dyes,AZ6+AZ5 with co-adsorbent chenodeoxycholic acid(CDCA)is presented.The power conversion efficiencies(PCEs)of 8.55%and 8.31%are obtained from DSSCs co-sensitized by AZ6(0.3 mmol/L)+AZ5(0.1 mmol/L)with CDCA concentration of 5 and 20 mmol/L in one step cocktail,respectively.The latter shows high stability in a period of 653 h under ambient conditions.
基金We thank the 111 Project(B21005)the National Natural Science Foundation of China(62174103)+2 种基金L.Ding thanks the National Key Research and Development Program of China(2022YFB3803300)the open research fund of Songshan Lake Materials Laboratory(2021SLABFK02)the National Natural Science Foundation of China(21961160720).
文摘Perovskite solar cell(PSC) is now a shining star in photovoltaics field[1].Benefiting from excellent optoelectronic properties of perovskite materials,the certified power conversion efficiency(PCE)of PSCs has reached 26.0%[2],showing great potential for commercialization.In essence,the efficiency of solar cells is determined by the radiative and nonradiative recombination of photogenerated charge carriers.The unfavorable nonradiative recombination mainly assisted by the trap states leads to severe charge carrier loss and thus unsatisfactory efficiency.
基金This research was sponsored by Key Technologies R&D Program of Shaanxi Province (Nos. 2014K10-06 and 2015XT-18), the National Natural Science Foundation of China (Nos. 51373092 and 21543012), the Funda-mental Research Funds for the Central Universities (Nos. GK201503038 and GK201501002), Program for Key Science & Technology Innovation Team of Shaanxi Province (No. 2015KCT-13), and the 111 Project (No. B14041).
文摘Highly effident metal-free, carbon-based, bi-functional electrocatalysts for the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) have attracted increased attention for use in electrochemical energy conversion systems, owing to their low cost and high activity. In this work, N-doped carbon nanocages (N-CCs) with a porous self-supported architecture and high specific surface area are synthesized by a facile interfacial assembly synthetic route. The materials are comprehensively characterized by scanning electron microscop36 transmission electron microscopy, nitrogen adsorption-desorption experiments, X-ray diffraction, and X-ray photoelectron spectroscopy. Cyclic voltammetry , chronoamperometry, and linear sweep voltammetry demonstrate that the as-prepared N-CC could serve as an effective metal-free electrocatalyst with excellent catalytic activity, long-term operation durability, and excellent methanol tolerance for the ORR in alkaline media. In the presence of 3 mM methanol, the half wave potential of the N-CCs for the ORR is 190 mV; this is more positive than that of the commercial Pt/C electrocatalyst. Meanwhile, the N-CCs also show an OER activity comparable to that of the commercial Ru/C electrocatalyst, revealing their bifunctional property.
基金The authors acknowledge the National Natural Science Foundation of China (Nos. 21576139, 21503111, 21376122, and 21273116), Jiangsu Provincial Natural Science Foundation of Jiangsu Province (No. BK20140926), Specialized Research Fund for the Doctoral Program of Higher Education (No. 20130202120010), the Key Science and Technology Program of Shaanxi Province, China (No. 2014K10-06), Fundamental Research Funds for the Central Universities (No. GK201503038), China Scholarship Council (CSC, 201506860013), University Postgraduate Research and Innovation Project in Jiangsu Province (No. KYZZ15_0213), National and Local Joint Engineering Research Center of Biomedical Functional Material, and a project funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions. The authors also thank John B. Goodenough of the university of Texas at Austin for his support and help.
文摘Catalysts for the oxygen reduction reaction (ORR) play an important role in fuel cells. Alternative non-precious metal catalysts with comparable ORR activity to Pt-based catalysts are highly desirable for the development of fuel cells. In this work, we report for the first time a spinel MnC0204/C ORR catalyst consisting of uniform MnC0204 nanoparticles cross-linked with two-dimensional (2D) porous carbon nanosheets (abbreviated as porous MnC0204/C nanosheets), in which glucose is used as the carbon source and NaC1 as the template. The obtained porous MnCo204/C nanosheets present the combined properties of an interconnected porous architecture and a large surface area (175.3 m2-g-1), as well as good electrical conductivity (1.15 x 102 S.cm-1). Thus, the as-prepared MnC0204/C nanosheets efficiently facilitate electrolyte diffusion and offer an expedite transport path for reactants and electrons during the ORR. As a result, the as-prepared porous MnC0204/C nanosheet catalyst exhibits enhanced ORR activity with a higher onset potential and current density than those of its counterparts, including pure MnC0204, carbon nanosheets, and Vulcan XC-72R carbon. More importantly, the porous MnC0204/C nanosheets exhibit a com- parable electrocatalytic activity but superior stability and tolerance toward methanol crossover effects than a high-performance Pt/C catalyst in alkaline medium. The synthetic strategy outlined here can be extended to other non- precious metal catalysts for application in electrochemical energy conversion.