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2D Ca/Nb-based perovskite oxide with Ta doping as highly efficient H_(2)O_(2)synthesis catalyst

Nano Research 2024年第6期17卷 4934-4942页

作者： Xingchen Yang Yang Gao Xiaohui Xu Wenqiang Xu Denghui Wang Bin Luo Dong Liu Tao Liang Bin Wang CAS Key Laboratory of Nanosystem and Hierarchical Fabrication National Center for Nanoscience and TechnologyBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Nanomaterials Centre School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnologythe University of QueenslandSt LuciaQLD 4072Australia State Key Laboratory of Organic–Inorganic Composites College of Chemical EngineeringCollege of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China Hangzhou Institute for Advanced Study University of Chinese Academy of SciencesHangzhou 310024China State Key Lab of Silicon Materials Zhejiang UniversityHangzhou 310027China

perovskite oxides(POs)are emerging as a class of highly efficient catalysts for reducing oxygen to H_(2)O.Although a rich variety of POs-based catalysts have been developed by tuning the complex composition,a highly efficient PO catalyst that is able to alter the reaction pathway from a 4e−process to a 2e−process for H_(2)O_(2)production has rarely been achieved.We modified the structure and composition of a Ca-and Nb-based PO material by realizing a uniform two-dimensional(2D)morphology and varied Ta doping,resulting in the 2D Ca_(2)Nb_(3−x)Ta_(x)O_(10)−(x=0,0.5,1,and 1.5)monolayer catalysts.The obtained catalysts exhibit a dominant 2e−pathway and show exceptional H_(2)O_(2)production efficiency.The typical Ca_(2)Nb_(2.5)Ta_(0.5)O_(10)−nanoflakes showed an onset potential of 0.735 V vs.reversible hydrogen electrode(RHE),a remarkably high selectivity over 95%across a wide range of 0.3-0.7 V,an impressively high Faradaic efficiency of 94%,and a notable H_(2)O_(2)productivity of 1571 mmol·gcat^(−1)·h^(−1).These findings highlight the great potential of 2D perovskite oxide nanoflakes as advanced electrocatalysts for 2e−oxygen reduction reaction.

关键词： perovskite oxide H_(2)O_(2) two-electron oxygen reduction reaction catalyst Ca_(2)Nb_(3-x)Ta_(x)O_(10)-nanoflakes

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

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能源化学:英文版 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 catalysts.Here,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 surface.This 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 layer.The 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 oxides.This 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 stacks.This 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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Nanoparticle Exsolution on perovskite oxides:Insights into Mechanism,Characteristics and Novel Strategies

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Nano-Micro Letters 2024年第2期16卷 312-346页

作者： Yo Han Kim Hyeongwon Jeong Bo‑Ram Won Hyejin Jeon Chan‑ho Park Dayoung Park Yeeun Kim Somi Lee Jae‑ha Myung Department of Materials Science and Engineering Incheon National UniversityIncheon 22012Republic of Korea

Supported nanoparticles have attracted considerable attention as a promising catalyst for achieving unique properties in numerous applications,including fuel cells,chemical conversion,and batteries.Nanocatalysts demonstrate high activity by expanding the number of active sites,but they also intensify deactivation issues,such as agglomeration and poisoning,simultaneously.Exsolution for bottomup synthesis of supported nanoparticles has emerged as a breakthrough technique to overcome limitations associated with conventional nanomaterials.Nanoparticles are uniformly exsolved from perovskite oxide supports and socketed into the oxide support by a one-step reduction process.Their uniformity and stability,resulting from the socketed structure,play a crucial role in the development of novel nanocatalysts.Recently,tremendous research efforts have been dedicated to further controlling exsolution particles.To effectively address exsolution at a more precise level,understanding the underlying mechanism is essential.This review presents a comprehensive overview of the exsolution mechanism,with a focus on its driving force,processes,properties,and synergetic strategies,as well as new pathways for optimizing nanocatalysts in diverse applications.

关键词： Supported nanoparticle Exsolution In situ growth Mechanism perovskite oxide Catalyst

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Efficient ammonia production over e_(g)-occupancy-optimized perovskite electrocatalysts

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Nano Research 2024年第6期17卷 4682-4686页

作者： Mingfa Chen Yu Zhang Fulong Liu Zhenbao Zhang Yuming Dong Yongfa Zhu Heqing Jiang Jiawei Zhu Key Laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi 214122China Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266101China School of Chemistry and Chemical Engineering Linyi UniversityLinyi 276005China Department of Chemistry Tsinghua UniversityBeijing 100084China

Renewable-energy-driven nitrate(NO_(3)^(−))electroreduction to ammonia(NH_(3))(NERA)has been an attractive technology for decarbonizing NH_(3)production and wastewater treatment.Improving NERA efficiency requires electrocatalysts that are earth-abundant and show fantastic performance.Here we report a semiempirical activity descriptor of eg occupancy(of surface B-site cations)for identifying inexpensive perovskite oxides with extremely high efficacy toward NERA.We establish the descriptor by systematic investigations of more than 10 perovskite oxides.These investigations demonstrate that their intrinsic NERA activities display a volcano-shaped dependence on eg occupancy and the optimized intrinsic activities are accessible at near-1 eg occupancies.This could plausibly be attributed to the favorable overlaps between surface adsorbates and vertically-oriented eg orbitals.More importantly,utilizing this descriptor,we predict a highly active,selective,and durable NERA electrocatalyst with a composition of Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3−δ)(BSCF).Because of its close-to-1 e_(g)occupancy(i.e.~1.2),the BSCF features a superior NH_(3)production rate of 0.12 g·h^(−1)·mg_(cat.)^(−1)(Faradaic efficiency of 97.8%)that is at top of the volcano plot,and substantially outperforms most NERA electrocatalysts reported in literature.

关键词： perovskite oxide nitrate electroreduction ammonia electrosynthesis eg occupancy

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Magnetic Behavior of Some Rare-Earth Transition-Metal perovskite oxide Systems

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Journal of Rare Earths 2004年第6期22卷 733-738页

作者： Kenji Yoshii Akio Nakamura Masaichiro Mizumaki Naoshi Ikeda Jun'ichiro Mizuki Japan Atomic Energy Research Institute Mikazuki Hyogo 679-5148 JapanJapan Atomic Energy Research Institute Tokai-mura Ibaraki 305-1195 JapanJapan Synchrotron Radiation Research Institute Mikazuki Hyogo 679-5198 JapanJapan Synchrotron Radiation Research Institute Mikazuki Hyogo 679-5198 JapanJapan Atomic Energy Research Institute Mikazuki Hyogo 679-5148 Japan

Magnetic properties were investigated for the rare-earth 3d-transition metal oxides with the perovskite structure. Intriguing magnetic phenomena were reviewed for a few systems:magnetization peak effect in the titanates, magnetization reversal in the chromites and metallic ferromagnetism in the cobaltites. The results suggest an important role of the rare-earth ions for the magnetic properties of such complex oxides.

关键词： perovskite oxide magnetic properties rare earth transition metal

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Effect of rare earth elements(La,Y,Pr)in multi-element composite perovskite oxide supports for ammonia synthesis

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Journal of Rare Earths 2021年第4期39卷 427-433页

作者： Wei Li Shuang Wang Jinping Li Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization College of Chemistry and Chemical EngineeringTaiyuan University of TechnologyTaiyuan 030024China College of Environmental Science and Engineering Taiyuan University of TechnologyJinzhong 030600China

A series of BaCe0_(3)modified with different rare earth elements(La,Y,Pr)were synthesized by coprecipitation and calcination and the effect of rare earth elements for catalytic ammonia synthesis under mild conditions was studied.The ammonia synthesis performance tests show that 2.5%Ru/BaCe_(0.9)La_(0.1)O_(3-δ)catalyst(All the percentages of Ru in this article are in mass fraction)exhibits the highest ammonia synthesis rate(34 mmol/(g·h))at 3 MPa,450℃,and no sign of deactivation after 100 h of reaction.H_(2)-TPR and XPS analyses indicate that the introduction of La increases the amount of oxygen vacancies of the catalyst,which is beneficial to increasing the electron density of Ru surface.HRTEM analysis shows that the Ru particle size is reduced greatly after La is introduced,which facilitates the catalyst generating more Bs-type sites(active sites of Ru species for N=N dissociation).CO_(2)-TPD analysis indicates that BaCe_(0.9)La_(0.1)O_(3-δ)has stronger basicity,which promotes electrons transfer from support to Ru.This work provides an effective method for design and synthesis of Ru-based multi-element composite perovskite oxide catalysts.

关键词： Ammonia synthesis Ru-based catalyst perovskite oxide Rare earth element(REE) Oxygen vacancies

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A bifunctional perovskite oxide catalyst:The triggered oxygen reduction/evolution electrocatalysis by moderated Mn-Ni co-doping

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Journal of Energy Chemistry 2021年第3期30卷 217-224页

作者： Jia Sun Lei Du Baoyu Sun Guokang Han Yulin Ma Jiajun Wang Hua Huo Pengjian Zuo Chunyu Du Geping Yin School of Chemistry and Chemical Engineering Harbin Institute of TechnologyHarbin 150001HeilongjiangChina

ABO_(3)-type perovskite oxides(e.g.,LaCoO_(3))with flexible and adjustable A-and B-sites are ideal model catalysts to unravel the relationship between the electronic structure and electrocatalytic activity(e.g.,oxygen reduction/evolution reactions,ORR/OER).It has been well understood in our recent work that the secondary metal dopant at B-site(e.g.,Mn in LaMn_(x)Co_(1-x)O_(3))can regulate the electronic structure and improve the ORR/OER activity.In this work,the Mn-Ni pairs are employed as the dual dopant in LaMn_(x)Ni_(y)Co_(z)O_(3)(x+y+z=1)catalysts toward bifunctional ORR and OER.The structure-property relationships between the triple metal B-site(Mn,Ni and Co)and the electrochemical performance are particularly investigated.Compared to the individual Mn doping(e.g.,LaMnCoO3(Mn:Co=1:3)catalyst),the dual Mn-Ni doping significantly improves the ORR mass activity@0.8 V by 1.54 times;meanwhile,the OER overpotential@10 mA cm^(-2) is reduced from 420 to 370 mV,and the OER current density at 1.55 V is increased by 2.43 times.Reasonably,the potential gap between EDRR@-1 mA cm^(-2) and EDER@10 mA cm^(-2) is achieved as only 0.76 V by using the optimal LaMn_(x)Ni_(y)Co_(z)O_(3)(x:y:z=1:2:3)catalyst.It is revealed that the dual Mn-Ni dopant efficiently optimizes electron structures of the LaMnNiCoO_(3)(1:2:3)catalyst,which not only decreases the e_(g) orbital electron number,but also modulates the O 2 p-band closer to the Femi level,accounting for the enhanced bifunctional activity.

关键词： perovskite oxide Bifunctional catalyst Mn-Ni dopant Oxygen reduction reaction Oxygen evolution reaction

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Thin Film of perovskite oxide with Atomic Scale p-n Junctions

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Chemical Research in Chinese Universities 2012年第3期28卷 379-381页

作者： HU Bin HUANG Ke-ke HOU Chang-min YUAN Hong-ming PANG Guang-sheng FENG Shou-hua State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012P.R.China

Thin films of perovskite manganese oxide Lao.66Ca0.29K0.05MnO3（LCKMO） on Au/ITO（ITO=indium tin oxide） substrates were prepared by off-axis radio frequency magnetron sputtering and characterized by X-ray diffrac- tion（XRD）, high-resolution transmission electron microscopy（HRTEM）, and conductive atomic force microscopy （C-AFM） at room temperature. The thin films with thickness ranged from 100 nm to 300 nm basically show cubic structures with a=0.3886 nm, the same as that of the raw material used, but the structures are highly modulated. C-AFM results revealed that the atomic scale p-n junction feature of the thin films was the same as that of the single crystals. The preparation of the thin films thus further confirms the possibility of their application extending from micrometer-sized single crystals to macroscopic thin film.

关键词： perovskite oxide Thin film Atomic scale p-n junction

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自组装FeRu双金属纳米催化剂在可逆固体氧化物电池中实现高效稳定的CO-CO_(2)相互转化

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Science China Materials 2024年第5期67卷 1471-1480页

作者：王晶张栋刘通徐安琪罗瑶胡学雷王瑶 Key Laboratory of Green Chemical Process of Ministry of Education Hubei Key Laboratory of Novel Reactor and Green Chemical TechnologySchool of Chemical Engineering and PharmacyWuhan Institute of TechnologyWuhan430205China School of Power and Mechanical Engineering Wuhan UniversityWuhan430072China

本文报道了一种适应于高效稳定的CO-CO_(2)相互转化的可逆固体氧化物电池(RSOC)相变燃料电极.该燃料电极由FeRu双金属纳米催化剂和Ruddlesden-Popper相Pr_(0.8)Sr_(1.2)Fe_(1-x-y)Ru_(x)Mo_(y)O_(4)氧化物复合而成(FeRu@PSFRM).固体氧化物燃料电池(SOFC)模式时,单电池800℃时的最大输出功率密度可以达到170 W cm^(-2);而在固体氧化物电解池(SOEC)模式下,800℃、1.3 V时电解池的电解电流密度达到-0.256 A cm^(-2).在SOFC-SOEC循环测试过程中,RSOC中CO-CO_(2)相互转化过程经历了“活化-稳定-衰退”三个明显阶段.幸运的是,性能衰退的燃料电极可通过“原位氧化-还原”处理实现性能再生,有效提升该电池的使用寿命.研究结果表明,原位脱溶形成的FeRu@PSFRM材料是一种极具应用潜力的燃料电极候选材料,以期实现高效稳定的CO-CO_(2)相互转化.

关键词： Ruddlesden-Popper oxide CO-CO_(2)conversion cycling test perovskite oxide reversible solid oxide cells distribution of relaxation times electrochemical impedance spectra fuel electrode

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Recent advances and perspectives of fluorite and perovskite-based dual-ion conducting solid oxide fuel cells

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Journal of Energy Chemistry 2021年第6期30卷 406-427,I0010页

作者： Jiafeng Cao Chao Su Yuexia Ji Guangming Yang Zongping Shao Institute of Materials Science and Engineering&School of Mathematics and Physics Anhui University of TechnologyMaanshan 243032AnhuiChina WA School of Mines:Minerals Energy and Chemical EngineeringCurtin UniversityPerth 6102Western AustraliaAustralia State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816JiangsuChina School of Energy and Power Jiangsu University of Science and TechnologyZhenjiang 212100JiangsuChina

High-temperature solid-state electrolyte is a key component of several important electrochemical devices,such as oxygen sensors for automobile exhaust control,solid oxide fuel cells(SOFCs) for power generation,and solid oxide electrolysis cells for H_(2) production from water electrolysis or CO_(2) electrochemical reduction to value-added chemicals.In particular,internal diffusion of protons or oxygen ions is a fundamental and crucial issue in the research of SOFCs,hypothetically based on either oxygen-ionconducting electrolytes or proton-conducting electrolytes.Up to now,some electrolyte materials based on fluorite or perovskite structure were found to show certain degree of dual-ion transportation capability,while in available electrolyte database,particularly in the field of SOFCs,such dual-ion conductivity was seriously overlooked.Actually,few concerns arising to the simultaneous proton and oxygen-ion conductivities in electrolyte of SOFCs inevitably induce various inadequate and confusing results in literature.Understanding dual-ion transportation behavior in electrolyte is indisputably of great importance to explain some unusual fuel cell performance as reported in literature and enrich the knowledge of solid state ionics.On the other hand,exploration of novel dual-ion conducting electrolytes will benefit the development of SOFCs.In this review,we provide a comprehensive summary of the understanding of dual-ion transportation in solid electrolyte and recent advances of dual-ion conducting SOFCs.The oxygen ion and proton conduction mechanisms at elevated temperature inside oxide-based electrolyte materials are first introduced,and then(mixed) oxygen ion and proton conduction behaviors of fluorite and perovskite-type oxides are discussed.Following on,recent advances in the development of dual-ion conducting SOFCs based on fluorite and perovskite-type single-phase or composite electrolytes,are reviewed.Finally,the challenges in the development of dual-ion conducting SOFCs are discussed and future prospects are

关键词： Dual-ion conduction Oxygen ion conduction Proton conduction Fluorite oxide perovskite oxide

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