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Constructing an OH−-enriched microenvironment on the electrode surface for natural seawater electrolysis

Nano Research 2024年第11期17卷 9483-9489页

作者： Jiaxin Guo Ruguang Wang Quanlu Wang Ruize Ma Jisi Li Erling Zhao Jieqiong Shan Tao Ling Key Laboratory for Advanced Ceramics and Machining Technology of Ministry of Education Institute of New-Energy School of Materials Science and Engineering Tianjin University Tianjin 300072 China Department of Chemistry City University of Hong Kong Hong Kong 999077 China

Powered by clean energy, the hydrogen fuel production from seawater electrolysis is a sustainable green hydrogen technology, however, chlorine corrosion and correlative oxidation reactions severely erode the catalysts. Our previous work demonstrates that direct seawater electrolysis without a desalination process and strong alkali addition can be realized by introducing a hard Lewis acid oxide on the catalyst surface to capture OH−. However, the criteria for selecting Lewis acid oxides and the origin of OH− enrichment in chlorine chemistry inhibition on the catalyst surface remain unexplored. Here, we compare the ability of a series of Lewis acid oxides with different acidity constants (pKa), including MnO_(2), Fe_(2)O_(3), and Cr_(2)O_(3), to enrich OH− on the Co3O4 anode catalyst surface. Comprehensive analyses suggest that the lower pKa value of the Lewis acid oxide, the higher concentration of OH− enriched on Co3O4 surface, and the lower Cl− concentration. As established correlation among pKa of Lewis acid oxide, OH− enrichment and Cl− repulsion provide direct guidance for future design of highly active, selective and durable catalysts for natural seawater electrolysis.

关键词： natural seawater electrolysis oxygen evolution reaction(OER)electrocatalyst Lewis acid OH−-enriched microenvironment chlorine chemistry

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Enhancing Structural Stability and Electrochemical Performance of Ultra-high Ni-rich Co-free Cathode via MgHPO_(4) Dual-functional Modification

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Chemical Research in Chinese Universities 2025年第2期41卷 333-342页

作者： LIN Huahui SHEN Yu WEI Li SONG Ran WU Fan WEI Peng YANG Zhenzhong REN Yurong QU Ke DING Zhengping Changzhou Key Laboratory of Intelligent Manufacturing and Advanced Technology for Power Battery Jiangsu Province Engineering Research Center of Intelligent Manufacturing Technology for the New Energy Vehicle Power BatterySchool of Materials Science and EngineeringChangzhou UniversityChangzhou 213164P.R.China Key Laboratory of Polar Materials and Devices(MOE) Shanghai Center of Brain-inspired Intelligent Materials and DevicesDepartment of ElectronicsEast China Normal UniversityShanghai 200241P.R.China

Ultra-high nickel layered cathodes(Ni≥95%)have emerged as prospective candidates for next-generation lithium-ion batteries(LIBs)due to their exceptional specific capacity and ***,the commercial application of these cathodes has been hindered by several challenges,including structural instability during cycling,high sensitivity to air,and slow Li+*** this research,a one-step modification strategy was developed to simultaneously achieve Mg doping and Li_(3)PO_(4)layer coating for the ultra-high nickel *** results demonstrated that Mg doping not only alleviates lattice strain changes during the H2–H3 phase transition(H2:the second hexagonal phase;H3:the third hexagonal phase)but also serves as a structural anchor,preventing Ni^(2+)migration and occupation within the Li *** Li_(3)PO_(4)surface coating layer acts as an electrochemical shield,protecting against interfacial side reactions and enhancing the Li+diffusion *** a result,the LiNi_(0.95)Mn_(0.05)O_(2) cathode,with both internal and external modifications,demonstrates significant improvement in cycling stability(85.7%capacity retention after 100 cycles)and Li^(+)transport performance(130.6 mA·h·g^(−1) at 10 C,1 C=189.6 mA·h·g^(−1)),providing a solid foundation for the further development and application of ultra-high nickel cathodes.

关键词： Lithium-ion battery Ni-rich Co-free cathode MgHPO_(4) Surface modification

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Efficient C-N coupling in electrocatalytic urea generation on copper carbonate hydroxide electrocatalysts

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Journal of Energy Chemistry 2024年第6期93卷 289-298,I0008页

作者： Yinuo Wang Yian Wang Qinglan Zhao Hongming Xu Shangqian Zhu Fei Yang Ernest P.Delmo Xiaoyi Qiu Chi Song Juhee Jang Tiehuai Li Ping Gao MDanny Gu Minhua Shao Advanced Materials Thrust The Hong Kong University of Science and Technology(Guangzhou)Guangzhou 511400GuangdongChina Department of Chemical and Biological Engineering The Hong Kong University of Science and TechnologyClear Water BayKowloonHong KongChina Department of Materials Science and Engineering Southern University of Science and Technology of Chin11088 Xueyuan BoulevardShenzhen 518055GuangdongChina Energy Institute and Chinese National Engineering Research Center for Control&Treatment of Heavy Metal PollutionThe Hong Kong University of Science and TechnologyKowloonHong KongChina Department of Chemistry City University of Hong KongTat Chee AvenueKowloonHong KongChina

Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of ***,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen *** thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~**** work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.

关键词： Copper carbonate hydroxide Co-reduction Urea generation C-N coupling DFT calculation

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Metal-organic framework-based single-atom electro-/ photocatalysts: Synthesis, energy applications, and opportunities

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Carbon Energy 2024年第1期6卷 1-43页

作者： Munir Ahmad Jiahui Chen Jianwen Liu Yan Zhang Zhongxin Song Shahzad Afzal Waseem Raza Liaqat Zeb Andleeb Mehmood Arshad Hussain Jiujun Zhang Xian-Zhu Fu Jing-Li Luo Shenzhen Key Laboratory of Energy Electrocatalytic Materials Guangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhenGuangdongChina College of Physics and Optoelectronic Engineering Shenzhen UniversityShenzhenGuangdongChina College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhenGuangdongChina Department of Environmental Engineering China Jiliang UniversityHangzhouZhejiangChina Institute for Advanced Study Shenzhen UniversityShenzhenGuangdongChina School of Bioengineering Dalian University of TechnologyDalianLiaoningChina College of Materials Science and Engineering Fuzhou UniversityFuzhouFujianChina Institute for Sustainable Energy Shanghai UniversityShanghaiChina

Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic ***,the high surface energy limits their synthesis,thus creating significant challenges for further *** 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 *** this perspective,this review thoroughly summarizes the previously reported methods and possible future approaches for constructing MOF-based(MOF-derived-supported and MOF-supported)***,MOF-based SAC's identification techniques are briefly assessed to understand their coordination environments,local electronic structures,spatial distributions,and catalytic/electrochemical reaction *** 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 *** light is also shed on the future development of this highly exciting field by highlighting the advantages and limitations of MOF-based SACs.

关键词： carbon energy generation MOF-derived-supported MOF-supported single atoms

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Atomic CoN_(3)S_(1) sites for boosting oxygen reduction reaction via an atomic exchange strategy

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Nano Research 2022年第3期15卷 1803-1808页

作者： Qianjun Zhi Rong Jiang Wenping Liu Tingting Sun Kang Wang Jianzhuang Jiang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China

It is vitally important to develop high-efficiency low-cost catalysts to boost oxygen reduction reaction(ORR)for renewable energy ***,an A-CoN_(3)S_(1)@C electrocatalyst with atomic CoN_(3)S_(1)active sites loaded on N,S-codoped porous carbon was produced by an atomic exchange *** constructed A-CoN_(3)S_(1)@C electrocatalyst exhibits an unexpected half-wave potential(0.901 V *** hydrogen electrode)with excellent durability for ORR under alkaline conditions(0.1 M KOH),superior to the commercial platinum carbon(20 wt.%Pt/C).The outstanding performance of A-CoN_(3)S_(1)@C in ORR is due to the positive effect of S atoms doping on optimizing the electron structure of the atomic CoN_(3)S_(1)active ***,the rechargeable zinc-air battery in which both A-CoN_(3)S_(1)@C and IrO_(2)were simultaneously served as cathode catalysts(A-CoN_(3)S_(1)@C&IrO_(2))exhibits higher energy efficiency,larger power density,as well as better stability,compared to the commercial Pt/C&IrO_(2)-based zinc-air *** present result should be helpful for developing lower cost and higher performance ORR catalysts which is expected to be used in practical applications in energy devices.

关键词： atomic sites oxygen reduction reaction CoN_(3)S_(1) zinc-air battery

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Enhanced photocatalytic performance of iron oxides@HTCC fabricated from zinc extraction tailings for methylene blue degradation:Investigation of the photocatalytic mechanism

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International Journal of Minerals,Metallurgy and materials 2023年第12期30卷 2364-2374页

作者： Yang Xue Xiaoming Liu Na Zhang Yang Shao Chunbao(Charles)Xu State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China School of Metallurgical and Ecological Engineering University of Science and Technology BeijingBeijing 100083China Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes National Laboratory of Mineral MaterialsSchool of Materials Science and TechnologyChina University of GeosciencesBeijing 100083China Department of Chemical&Biochemical Engineering Western UniversityLondonON N6A 5B9Canada

Photocatalytic processes are efficient methods to solve water contamination problems,especially considering dyeing wastewater ***,high-efficiency photocatalysts are usually very expensive and have the risk of heavy metal ***,an iron oxides@hydrothermal carbonation carbon(HTCC)heterogeneous catalyst was prepared by our group through co-hydrothermal treatment of carbohydrates and zinc extraction tailings of converter ***,the catalytic performance of the iron oxides@HTCC was verified by a nonbiodegradable dye,methylene blue(MB),and the catalytic mechanism was deduced from theoretical simulations and spectroscopic *** iron oxides@HTCC showed an excellent synergy between photocatalysis and Fenton-like *** visible-light illumination,the iron oxides@HTCC could be excited to generate electrons and holes,reacting with H_(2)O_(2)to produce·OH radicals to oxidize and decompose organic *** removal efficiency of methylene blue over iron oxides@HTCC at 140 min was 2.86 times that of *** enhanced catalytic performance was attributed to the advantages of iron oxides modification:(1)promoting the excitation induced by photons;(2)improving the charge ***,the iron oxides@HTCC showed high catalytic activity in a wide pH value range of 2.3-10.4,and the MB removal efficiency remained higher than 95% after the iron oxides@HTCC was recycled 4 *** magnetically recyclable iron oxides@HTCC may provide a solution for the treatment of wastewater from the textile industry.

关键词： photocatalysis photo-Fenton reaction methylene blue degradation tailings utilization

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Fundamental Understanding on Selenium Electrochemistry:From Electrolytic Cell to advanced Energy Storage

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Energy & Environmental materials 2024年第3期7卷 236-256页

作者： Jiguo Tu Cheng Chang Jingxiu Wang Haiping Lei R.Vasant Kumar Mingyong Wang Shuqiang Jiao State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China School of Chemical Engineering The University of AdelaideAdelaideSA 5005Australia School of Metallurgical and Ecological Engineering University of Science and Technology BeijingBeijing 100083China Department of Materials Science and Metallurgy University of CambridgeCambridge CB30FSUK

Selenium(Se),as an important quasi-metal element,has attracted much attention in the fields of thin-film solar cells,electrocatalysts and energy storage applications,due to its unique physical and chemical ***,the electrochemical behavior of Se in different systems from electrolytic cell to battery are complex and not fully *** this article,we focus on the electrochemical processes of Se in aqueous solutions,molten salts and ionic liquid electrolytes,as well as the application of Se-containing materials in energy ***,the electrochemical behaviors of Se-containing species in different systems are comprehensively summarized to understand the complexity of the kinetic processes and guide the Se ***,the relationship between the deposition conditions and resulting structure and morphology of electrodeposited Se is discussed,so as to regulate the morphology and composition of the ***,the advanced energy storage applications of Se in thin-film solar cells and secondary batteries are reviewed,and the electrochemical reaction processes of Se are systematically comprehended in monovalent and multivalent metal-ion *** on understanding the fundamental electrochemistry mechanism,the future development directions of Se-containing materials are considered in view of the in-depth review of reaction kinetics and energy storage applications.

关键词： electrochemical behaviors electrodeposition electrolytes energy storage selenium

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A novel oxidation-resistible Mg@Ni foam material for safe,efficient,and controllable hydrogen generation

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Journal of Magnesium and Alloys 2024年第10期12卷 4063-4074页

作者： Jingru Liu Busheng Zhang Haiping Yu Tengfei Li Mingjun Hu Jun Yang Beijing Institute of Nanoenergy and Nanosystems Chinese Academy of SciencesBeijing 101400China College of Materials Science and Opto-Electronic Technology University of Chinese Academy of SciencesBeijing 100049China Department of Mechanical and Materials Engineering Western UniversityLondonOntarioN6A 5B9Canada School of Nanoscience and Technology University of Chinese Academy of SciencesBeijing 100049China School of Materials Science and Engineering Beihang UniversityBeijing 100191China ShenSi Lab Shenzhen Institute for Advanced StudyUniversity of Electronic Science and Technology of ChinaShenzhen 518110China

As a promising in-situ hydrogen generation material,magnesium(Mg)has been seeking a promotion in its hydrogen generation *** the specific surface area,for example,replacing the Mg bulk using Mg powder,can greatly increase the hydrogen generation property,but it brings a high explosion risk,a difficulty in controlling the hydrogen generation,and an oxidation *** this work,we prepare a novel Mg@Ni foam material with Mg deposits on Ni foam by a physical vapor deposition *** Ni foam not only increases the hydrolysis reaction areas of Mg by improving its specific surface area,but also kinetically accelerates the hydrolysis reaction rate of Mg by forming a uniform Mg-Ni galvanic *** a result,the Mg@Ni foam material realizes a near-theoretical hydrogen generation amount of Mg and a hydrogen generation rate significantly higher than those realized by the bulk Mg-based *** Mg@Ni foam material with the excellent hydrogen generation property is also free from explosion risk,easy to be controlled,and resistible to oxidation.A hydrogen fuel cell powered by the hydrogen generated by the Mg@Ni foam material can yield a steady voltage and run a small car for a long distance.

关键词： Mg@Ni foam material Physical vapor deposition Hydrogen generation

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Rapid and durable oxygen reduction reaction enabled by a perovskite oxide with self-cleaning surface

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Journal of Energy Chemistry 2023年第8期83卷 333-340,I0010页

作者： Shengli Pang Yifan Song Meng Cui Xin Tang Chao Long Lingfeng Ke Gongmei Yang Ting Fang Yong Guan Chonglin Chen Institute for Advanced Materials School of Materials Science and EngineeringJiangsu UniversityZhenjiang 212013JiangsuChina Department of Physics and Astronomy The University of Texas at San AntonioSan AntonioTX 78249USA College of Material Science and Engineering Guilin University of TechnologyGuilin 541004GuangxiChina National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230026AnhuiChina

The growth of electrochemically inert segregation layers on the surface of solid oxide fuel cell cathodes has become a bottleneck restricting the development of perovskite-structured oxygen reduction ***,we report a new discovery in which enriched Ba and Fe ions on the near-surface of Nd_(1/2)Ba_(1/2)Co_(1/3)Fe_(1/3)Mn_(1/3)O_(3-δ)spontaneously agglomerate into dispersed Ba_(5)Fe_(2)O_(8) nanoparticles and maintain a highly active and durable perovskite structure on the *** unique surface selfcleaning phenomenon is related to the low average potential energy of Ba_(5)Fe_(2)O_(8),which is grown on the near-surface *** electrochemically inert Ba_(5)Fe_(2)O_(8) segregation layer on the near-surface of the perovskite catalyst achieves self-cleaning by regulating the formation energy of enriched metal *** self-cleaned perovskite surface exhibits an ultrafast oxygen exchange rate,high catalytic activity for the oxygen reduction reaction,and good adaptability to the actual working conditions of solid oxide fuel cell *** study paves a new way for overcoming the stubborn problem of perovskite catalyst surface deactivation and enriches the scientific knowledge of surface catalysis.

关键词： Surface chemistry Energy materials Electrocatalysis Perovskite oxide Oxygen reduction reaction Solid oxide fuel cells

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Bifunctional self-segregated electrolyte realizing high-performance zinc-iodine batteries

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InfoMat 2024年第12期6卷 112-123页

作者： Xueting Hu Zequan Zhao Yongqiang Yang Hao Zhang Guojun Lai Bingan Lu Peng Zhou Lina Chen Jiang Zhou School of Materials Science and Engineering Hunan Provincial Key Laboratory of Electronic Packaging and Advanced Functional MaterialsCentral South UniversityChangshaHunanthe people's Republic of China Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityHong Kong SARthe people's Republic of China Department of Chemical Engineering Massachusetts Institute of TechnologyCambridgeMassachusettsUSA School of Physics and Electronics Hunan UniversityChangshaHunanthe people's Republic of China Hunan Provincial Key Defense Laboratory of High Temperature Wear-Resisting Materials and Preparation Technology Hunan University of Science and TechnologyXiangtanHunanthe people's Republic of China School of Materials Science and Engineering Harbin Institute of Technology(Shenzhen)ShenzhenGuangdongthe people's Republic of China

Static rechargeable zinc-iodine(Zn-I_(2))batteries are superior in safety,costeffectiveness,and sustainability,giving them great potential for large-scale energy storage ***,the shuttle effect of polyiodides on the cathode and the unstable anode/electrolyte interface hinder the development of Zn-I_(2)***,a self-segregated biphasic electrolyte(SSBE)was proposed to synergistically address those *** strong interaction between polyiodides and the organic phase was demonstrated to limit the shuttle effect of ***,the hybridization of polar organic solvent in the inorganic phase modulated the bonding structure,as well as the effective weakening of water activity,optimizing the interface during zinc *** a result,the Zn-I_(2)coin cells performed a capacity retention of nearly 100%after 4000 cycles at 2 mA cm^(-2).And a discharge capacity of 0.6 Ah with no degradation after 180 cycles was achieved in the pouch cell.A photovoltaic energy storage battery was further achieved and displayed a cumulative capacity of 5.85 *** successfully designed energy storage device exhibits the application potential of Zn-I_(2)batteries for stationary energy storage.

关键词： bifunctional modification self-segregated electrolyte shuttle-free zinc-iodine batteries

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