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A self-powered system to electrochemically generate ammonia driven by palladium single atomelectrocatalyst

SusMat 2024年第5期4卷 178-188页

作者： Hao Hu Shuyuan Pan Zhiyong Ma Kaiyi Liu Yi Li Haifeng Bao Chengwei Deng Fang Luo Zehui Yang State Key Laboratory of New Textile Materials&Advanced Processing Technology College of Materials Science and EngineeringWuhan Textile UniversityWuhanChina Faculty of Materials Science and Chemistry China University of GeosciencesWuhanChina Shaanxi Coal Chemical Industry Technology Research Institute Co. Ltd.Xi’anChina State Key Laboratory of Space Power-Sources Technology Shanghai Institute of Space Power SourcesShanghaiChina Hubei Key Laboratory for New Textile Materials and Applications Wuhan Textile UniversityWuhanChina

The utilization of single atoms(SAs)as trifunctional electrocatalyst for nitro-gen reduction,oxygen reduction,and oxygen evolution reactions(NRR,ORR,and OER)is still a formidable ***,we devise one-pot synthesized palladium SAs stabilized on nitrogen-doped carbon palladium SA electrocat-alyst(Pd-SA/NC)as efficient trifunctional electrocatalyst for NRR,ORR,and ***-SA/NC performs a robust catalytic activity toward NRR with faradaic efficiency of 22.5%at-0.25 V versus reversible hydrogen electrode(RHE),and the relative Pd utilization efficiency is enhanced by 17-fold than Pd-NP/*** addition,the half-wave potential reaches 0.876 V versus RHE,amounting to a 58-time higher mass activity than commercial Pt/***,the overpotential at 10 mA cm-2 is as low as 287 mV for Pd-SA/NC,outperforming the commer-cial IrO2 by 360 times in turnover frequency at 1.6 V versus ***,the assembled rechargeable zinc-air battery(ZAB)achieves a maximum power den-sity of 170 mW cm-2,boosted by 2.3 times than Pt/C–*** constructed ZABs efficiently power the NRR-OER system to electrochemically generate ammonia implying its superior trifunctionality.

关键词： nitrogen reduction reaction oxygen evolution reaction oxygen reduction reaction single atom

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Chiral electrolytes for rechargeable metal batteries

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Journal of Energy Chemistry 2025年第3期102卷 834-841页

作者： Lan-Qing Wu Yu-Jie Ning Zhen-Yu Fan Zhe Li Kun Li Jia Li Shuang-Xin Ren Dubin Huang Yang Yang Weiwei Xie Huan Wang Qing Zhao Frontiers Science Center for New Organic Matter Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)State Key Laboratory of Advanced Chemical Power SourcesCollege of ChemistryNankai UniversityTianjin 300071China Beijing Golden Feather New Energy Technology Co. LtdBeijing 100080China

Charge transfer at the liquid(electrolyte)-solid(metal)interfaces is of fundamental importance to metal electrochemical deposition that further determines the reversibility and kinetics of energy-dense rechargeable metal batteries(RMBs).We demonstrate the fast charge transfer at the electrolyte-metal interfaces for lithium metal by designing and synthesizing electrolytes with chiral solvents:R(or S)-1,2-dimethoxy pro pane(R-DMP or S-DMP)and R(or S)-4-methyl-1,3-dioxolane(R-MDOL or S-MDOL).The chiral-induced spin selectivity is considered to produce spin-polarized metal surfaces,enabling the improvement in charge transfer rate and *** deposited Li metal in chiral electrolytes shows smooth and uniform morphologies,as well as high initial(>95%)and average(~99.2%)Coulombic efficiency for Li metal stripping/plating process,thus prolonging the life-span of batteries using thin lithium anode(50μm)to 400 cycles till 80%capacity *** work provides a distinct approach to regulate metal deposition beyond the limitation of ion de-solvation.

关键词： Chiral ether electrolytes Electrode kinetics Li metal batteries Metal deposition Solvation structures

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Key role of electron accessibility at the noble metal-free catalytic interface in hydrogen evolution reaction

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Nano Research 2024年第4期17卷 2538-2545页

作者： Dongchen Han Nanxing Gao Yuyi Chu Zhaoping Shi Ying Wang Junjie Ge Meiling Xiao Changpeng Liu Wei Xing State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Jilin Province Key Laboratory of Low Carbon Chemical Power Sources Changchun 130022China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The reactant concentration at the catalytic interface holds the key to the activity of electrocatalytic hydrogen evolution reaction(HER),mainly referring to the capacity of adsorbing hydrogen and electron *** hydrogen adsorption free energy(ΔGH)as a reactivity descriptor,the volcano curve based on Sabatier principle is established to evaluate the hydrogen evolution activity of ***,the role of electron as reactant received insufficient attention,especially for noble metal-free compound catalysts with poor conductivity,leading to cognitive gap between electronic conductivity and apparent catalytic *** we successfully construct a series of catalyst models with gradient conductivities by regulating molybdenum disulfide(MoS_(2))electronic bandgap via a simple solvothermal *** demonstrate that the conductivity of catalysts greatly affects the overall catalytic *** further elucidate the key role of intrinsic conductivity of catalyst towards water electrolysis,mainly concentrating on the electron transport from electrode to catalyst,the electron accumulation process at the catalyst layer,and the charge transfer progress from catalyst to *** and experimental evidence demonstrates that,with the enhancement in electron accessibility at the catalytic interface,the dominant parameter governing overall HER activity gradually converts from electron accessibility to combination of electron accessibility and hydrogen adsorbing *** results provide the insight from various perspective for developing noble metal-free catalysts in electrocatalysis beyond HER.

关键词： conductivity molybdenum disulfide catalytic interface electron accessibility hydrogen evolution charge transfer.

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Uniform Ag_(6)Mo_(10)O_(33) meso/nanowires:High-efficient fabrication,novel growth mechanism,and reversibly high-energy sodium-ion battery

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Nano Research 2025年第4期18卷 189-198页

作者： Yuqing Yang Juan Liu Meiqi Zhang Qing Wang Ziqing Gui Xucheng Gu Chunsheng Li Yan Sun Yuxuan Sun Lianghuan Qin Yuzhen Zhao Wanzheng Lu Xiaofang Xu Xufeng Wang Key Laboratory of Advanced Electrode Materials for Novel Solar Cells for Petroleum and Chemical Industry of China School of Chemistry and Life SciencesSuzhou University of Science and TechnologySuzhou 215009China Xi’an Key Laboratory of Advanced Photo-electronics Materials and Energy Conversion Device School of Electronic InformationXijing UniversityXi’an 710123China School of Safety Science and Engineering Changzhou UniversityChangzhou 213164China Suzhou Key Laboratory of Biophotonics School of Optical and Electronic InformationSuzhou City UniversitySuzhou 215104China State Key Laboratory of Advanced Chemical Power Sources Guizhou Meiling Power Sources Co.LtdZunyi 563003China

Silver molybdate(Ag_(6)Mo_(10)O_(33))exhibits excellent catalytic properties and photocatalytic degradation owing to its unique chemical and structural characteristics,but its prospective applications in electrochemistry energy storage have not received sufficient ***,the Ag_(6)Mo_(10)O_(33) meso/nanowires with superior morphological characteristics are fabricated employing a high-efficient microwave irradiation ***,the novel synthesizing mechanism of ultralong Ag_(6)Mo_(10)O_(33) mesowires is also proved to be a“self-assembly-dissolution-recrystallization-Ostwald-ripening”process,by exploring through the parallel experiments on the dramatic alterations in topology and size of Ag_(6)Mo_(10)O_(33) at continuous reaction ***,the properties of the ultralong uniform Ag_(6)Mo_(10)O_(33) mesowires for the sodium storage are investigated via cyclic voltammetry,electrochemical impedance spectroscopy and galvanostatic ***,these as-obtained Ag_(6)Mo_(10)O_(33) mesowires exhibit an outstanding initial capacity(1587.9 mAh·g^(-1)),a remarkable specific capacity for the second cycle(817.9 mAh·g^(-1)),and an excellent reversible capacity(551.5 mAh·g^(-1) after 30 cycles).The superior electrochemical properties of the nanoscaled silver molybdate are ascribed to the lower charge transfer resistance due to the microstructure of the smallest size Ag_(6)Mo_(10)O_(33) nanosheets that exhibit a thickness of around 5 nm,which can provide a great contact with the electrolyte,facilitating the rapid diffusion of sodium ions at the electrode/electrolyte interface and the rapid transport of sodium ions within the electrode ***,the proposed synthetic strategy and achieved deep insights will stimulate the development of Ag_(6)Mo_(10)O_(33) for high-safety and long-life sodium ion batteries.

关键词： sodium-ion batteries self-assembly-dissolution-recrystallization-Ostwald-ripening fabricating mechanism microwave irradiation fabrication Ag_(6)Mo_(10)O_(33)meso/nanowires energy storage and conversion

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Micropores regulating enables advanced carbon sphere catalyst for Zn-air batteries

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Green Energy & Environment 2023年第1期8卷 308-317页

作者： Jingsha Li Shijie Yi Ranjusha Rajagopalan Zejie Zhang Yougen Tang Haiyan Wang Hunan Provincial Key Laboratory of Chemical Power Sources Hunan Provincial Key Laboratory of Efficient and Clean Utilization of Manganese ResourcesCollege of Chemistry and Chemical EngineeringCentral South UniversityChangsha410083China Institute of Materials Science and Devices Suzhou University of Science and TechnologySuzhou215011China

Energy conversion technologies like fuel cells and metal-air batteries require oxygen reduction reaction(ORR)electrocatalysts with low cost and high catalytic ***,N-doped carbon spheres(N-CS)with rich micropore structure have been synthesized by a facile two-step method,which includes the polymerization of pyrrole and formaldehyde and followed by a facile pyrolysis *** the preparation,zinc chloride(ZnCl2)was utilized as a catalyst to promote polymerization and provide a hypersaline *** addition,the morphology,defect content and activity area of the resultant N-CS catalysts could be regulated by controlling the content of *** optimum N-CS-1 catalyst demonstrated much better catalytic activity and durability towards ORR in alkaline conditions than commercial 20 wt%Pt/C catalysts,of which the half-wave potential reached 0.844 V *** applied in the Zn-air batteries as cathode catalysts,N-CS-1 showed a maximum power density of 175 mW cm^(-2) and long-term discharging stability of over 150 h at 10 mA cm^(-2),which outperformed 20 wt%Pt/*** excellent performance could be due to its ultrahigh specific surface area of 1757 m2 g1 and rich micropore channels ***,this work provides an efficient method to synthesize an ultrahigh surface porous carbon material,especially for catalyst application.

关键词： Zn-air batteries Oxygen reduction reaction N-doped carbon spheres Micropores Ultrahigh specific surface

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Research progress in failure mechanisms and electrolyte modification of high-voltage nickel-rich layered oxide-based lithium metal batteries

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InfoMat 2024年第2期6卷 57-75页

作者： Jiandong Liu Xinhong Hu Shihan Qi Yurong Ren Yong Li Jianmin Ma School of Chemistry Tiangong UniversityTianjinthe People's Republic of China School of Physics and Electronics Hunan UniversityChangshathe People's Republic of China School of Materials Science and Engineering Jiangsu Collaborative Innovation Center of Photovoltaic Science and EngineeringChangzhou UniversityChangzhouthe People's Republic of China State Key Laboratory of Space Power-Sources Technology Shanghai Institute of Space Power SourcesShanghaithe People's Republic of China

High-voltage nickel(Ni)-rich layered oxide-based lithium metal batteries(LMBs)exhibit a great potential in advanced batteries due to the ultra-high energy ***,it is still necessary to deal with the challenges in poor cyclic and thermal stability before realizing practical application where cycling life is *** many improved strategies,mechanical and chemical stability for the electrode electrolyte interface plays a key role in addressing these ***,extensive effort has been made to address the challenges of electrode-electrolyte *** this progress,the failure mechanism of Ni-rich cathode,lithium metal anode and electrolytes are reviewed,and the latest breakthrough in stabilizing electrode-electrolyte interface is also ***,the challenges and future research directions of Ni-rich LMBs are put forward.

关键词： electrode-electrolyte interface electrolyte modification failure mechanisms high voltage lithium metal anode nickel-rich layered oxide cathode

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Ultra-stable Pt_(5)La intermetallic compound towards highly efficient oxygen reduction reaction

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Nano Research 2023年第2期16卷 2035-2040页

作者： Siyuan Zhu Liting Yang Jingsen Bai Yuyi Chu Jie Liu Zhao Jin Changpeng Liu Junjie Ge Wei Xing State Key Laboratory of Electroanalytical Chemistry Laboratory of Advanced Power SourcesChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied Chemistry and Engineering University of Science and Technology of ChinaUniversity of Science and Technology of China(USTC)Hefei 230026China Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalian 116023China

Designing feasible electrocatalysts towards oxygen reduction reaction(ORR)requires advancement in both activity and stability,where attaining high stability is of extreme importance as the catalysts are expected to work efficiently under frequent start-up/shut down circumstances for at least several thousand *** platinum with early transition metals(i.e.,Pt–La alloy)is revealed as efficient catalysts construction strategy to potentially satisfy these *** we report a Pt5La intermetallic compound synthesized by a novel and facile *** to the strong electronic interactions between Pt and La,the resultant Pt5La alloy catalyst exhibits enhanced activity with half wave of 0.92 V and mass activity of 0.49 A·mgPt^(−1),which strictly follows the 4e transfer *** importantly,the catalyst performs superior stability during 30,000 cycles of accelerated stressed test(AST)with mass activity retention of 93.9%.This study provides new opportunities for future applications of Pt-rare earth metal alloy with excellent electrocatalytic properties.

关键词： oxygen reduction reaction intermetallic compound rare earth metal electrocatalysis

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Revealing the true origin of size-dependent Pd/C catalytic behavior towards formic acid decomposition

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Chinese Chemical Letters 2023年第1期34卷 457-460页

作者： Qinglei Meng Xian Wang Meiling Xiao Zhao Jin Junjie Ge Changpeng Liu Wei Xing Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of Science and Technology of China Hefei 230026China Jilin Province Key Laboratory of Low Carbon Chemical Power Sources Changchun 130022China State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Formic acid decomposition(FAD)is considered a promising hydrogen production route to facilitate the ambient storage and on demand release of hydrogen *** optimize the catalysts for FAD,efforts have been paid to explore the underlying reason for the varied catalytic activity among catalysts with similar composition but differed ***,such endeavors are highly challenging due to the deeply intermingled effects of electronic structure,particle size,and facets,***,to separately evaluate the respective effects of these factors,a series of catalysts with the same surface electronic structure and different particle size was prepared by cation dipole adjustment *** performance and characterization results showed that the catalysts with different sizes and facets exhibited similar intrinsic activity with deviation of less than 5%.However,they showed 252%deviation of site stability,indicating that only the optimized electronic structure could enhance the intrinsic activity and a smaller particle size could extend the catalyst’s life.

关键词： Hydrogen production Formic acid Catalyst deactivation Size effect Facets effect

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Design of Ti_(2)AlC/YSZ TBCs for more efficient in resisting CMAS attack

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Journal of Advanced Ceramics 2023年第9期12卷 1712-1730页

作者： Lei Guo Yanyan Li Guang Li School of Materials Science and Engineering Tianjin UniversityTianjin 300072China Tianjin Key Laboratory of Advanced Joining Technology Key Lab of Advanced Ceramics and Machining TechnologyMinistry of EducationTianjin 300072China Shanghai Institute of Space Power-Sources Shanghai 200240China

Ti_(2)AlC has been demonstrated as the promising protective layer material for thermal barrier coatings(TBCs)against calcium-magnesium-alumina-silicate(CMAS)*** this study,the reliability of Ti_(2)AlC coatings against the CMAS corrosion was explored,and new Ti_(2)AlC/YSZ TBCs more efficiently resistant to CMAS were *** fabricated Ti_(2)AlC coatings inevitably contain some impurity phases(TiC and Al2Ti3),the contents of which were minimized by optimizing the spraying *** tests revealed that Ti_(2)AlC/YSZ TBCs yielded higher resistance to the CMAS attack than YSZ TBCs,but with long-term exposure to CMAS,the Ti_(2)AlC protective coating exhibited microstructure degradation due to the presence of the impurity phases,which caused the formation of a layer mixed with Al_(2)O_(3)and TiO_(2)rather than a continuous compact Al_(2)O_(3)layer on the ***-oxidation schemes were designed in air or with a controlled oxygen partial pressure,which revealed that the pre-oxidation at an oxygen partial pressure of~630 Pa could promote a continuous Al_(2)O_(3)layer formed on the Ti_(2)AlC protective coating ***,a vacuum heat treatment at 867℃for 10 h before pre-oxidation was beneficial for the formation of the compact Al_(2)O_(3)*** the above scheme design,new Ti_(2)AlC/YSZ TBCs were obtained,which had reduced impurity phase contents and a pre-oxide layer with an ideal structure on the *** TBCs exhibit higher microstructure stability exposed to CMAS and more efficient CMAS resistance.

关键词： thermal barrier coatings(TBCs) calcium-magnesium-alumina-silicate(CMAS) Ti_(2)AlC/YSZ pre-oxidation design corrosion resistance mechanisms

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Identification of active sites and synergistic effect in multicomponent carbon-based Ru catalysts during electrocatalytic hydrogen evolution

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Nano Research 2023年第1期16卷 166-173页

作者： Rongpeng Ma Xian Wang Xiaolong Yang Yang Li Changpeng Liu Junjie Ge Wei Xing State Key Laboratory of Electroanalytical Chemistry Laboratory of Advanced Power SourcesChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalian 116023China

Single atom catalysts(SACs)were reported to demonstrate exciting catalytic features for a number of reactions,including hydrogen evolution reaction(HER).However,the true role of these single atom sites in catalysts remains elusive,particularly for those prepared via pyrolysis,where the formation of active nanoparticle counterparts is often *** we report a Ru based catalyst(Ru embedded in N doped carbon spheres(Ru/NPCS))comprising of both Ru nanoclusters and Ru single sites,who demonstrates activity exceeding Pt catalyst and mass activity among the best of the Ru based catalysts under acidic *** integration of proton exchange membrane water electrolysis with Ru/NPCS as a cathode exhibited an excellent hydrogen generation activity and extraordinary stability(during 120 h of electrolysis)with a 1/48 Ru loading(16.5μgRu·cm^(−2))of a commercial 20%Pt/C *** precisely tailoring the dispersion status of the catalysts,we reveal that while ruthenium nanoclusters actively catalyze HER via Volmer–Tafel mechanism,the Ru SACs barely catalyze HER,with H*adsorption difficult to ***,no synergy between Ru SACs and Ru cluster is revealed,meaning the Ru SACs act as a spectator rather than active species during H2 evolution.

关键词： hydrogen evolution reaction single atom catalysts nanoclusters no synergy

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