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Ultrafast metal oxide reduction at Pd/PdO_(2) interface enables onesecond hydrogen gas detection under ambient conditions

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Nano Research 2023年第1期16卷 1149-1157页

作者： Xin Geng Shuwei Li Zhi Mei Dongsheng Li Liang Zhang Long Luo Department of Chemistry Wayne State UniversityDetroitMI 48202USA Center for Combustion Energy Tsinghua UniversityBeijing 100084China School of Vehicle and Mobility Tsinghua UniversityBeijing 100084China State Key Laboratory of Automotive Safety and Energy Beijing 100084China Physical and Computational Sciences Directorate Pacific Northwest National LaboratoryRichlandWA 99352USA

Here,we report a Pd/PdO_(x) sensing material that achieves 1-s detection of 4% H_(2) gas(i.e.,the lower explosive limit concentration for H_(2))at room temperature in air.The Pd/PdO_(x) material is a network of interconnected nanoscopic domains of Pd,PdO,and PdO_(2).Upon exposure to 4% H_(2),PdO and PdO_(2) in the Pd/PdO_(x) are immediately reduced to metallic Pd,generating over a>90% drop in electrical resistance.The mechanistic study reveals that the Pd/PdO_(2) interface in Pd/PdOx is responsible for the ultrafast PdO_(x) reduction.Metallic Pd at the Pd/PdO_(2) interface enables fast H_(2) dissociation to adsorbed H atoms,significantly lowering the PdO2 reduction barrier.In addition,control experiments suggest that the interconnectivity of Pd,PdO,and PdO2 in our Pd/PdO_(x) sensing material further facilitates the reduction of PdO,which would otherwise not occur.The 1-s response time of Pd/PdO_(x) under ambient conditions makes it an excellent alarm for the timely detection of hydrogen gas leaks.

关键词： metal oxide reduction Pd/PdO_(2) interface 1-s H_(2)gas detection ambient conditions

Defect and interface engineering for electrochemical nitrogen reduction reaction under ambient conditions

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Journal of Energy Chemistry 2022年第2期31卷 448-468页

作者： Dongxue Guo Shuo Wang Jun Xu Wenjun Zheng Danhong Wang TKL of Metal and Molecule Based Material Chemistry School of Materials Science and EngineeringCollege of ChemistryNankai UniversityTianjin 300350China Center for Rare Earth and Inorganic Functional Materials Tianjin Key Lab for Rare Earth Materials and ApplicationsNational Institute for Advanced MaterialsSchool of Materials Science and EngineeringNankai UniversityTianjin 300350China

Electrochemical nitrogen reduction reaction(e-NRR)under ambient conditions is an emerging strategy to tackle the hydrogen-and energy-intensive operations for traditional Haber-Bosch process in industrial ammonia(NH_(3))synthesis.However,the e-NRR performance is currently impeded by the inherent inertness of N_(2) molecules,the extremely slow kinetics and the overwhelming competition from the hydrogen evolution reaction(HER),all of which cause unsatisfied yield and ammonia selectivity(Faradaic efficiency,FE).Defect and interface engineering are capable of achieving novel physical and chemical properties as well as superior synergistic effects for various electrocatalysts.In this review,we first provide a general introduction to the NRR mechanism.We then focus on the recent progress in defect and interface engineering and summarize how defect and interface can be rationally designed and functioned in NRR catalysts.Particularly,the origin of superior NRR catalytic activity by applying these approaches was discussed from both theoretical and experimental perspectives.Finally,the remaining challenges and future perspectives in this emerging area are highlighted.It is expected that this review will shed some light on designing NRR electrocatalysts with excellent activity,selectivity and stability.

关键词： Nitrogen reduction Electrocatalysis Defect engineering Interface engineering ambient conditions

维普期刊数据库

Rock-salt and helix structures of silver iodides under ambient conditions

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National Science Review 2019年第4期6卷 767-774页

作者： Hongyang Huang Jinying Zhang Yifan Zhang Chengcheng Fu Jialiang Huang Yonghong Cheng Chunming Niu Xinluo Zhao Hisanori Shinohara State Key Laboratory of Electrical Insulation and Power Equipment Center of Nanomaterials for Renewable Energy (CNRE) School of Electrical EngineeringXi'an Jiaotong University Department of Physics Shanghai University Department of Chemistry and Institute for Advanced Research Nagoya University

Many different phase structures have been discovered for silver iodides. The β and γ phases were found to be the most common ones at ambient conditions, while the rock-salt phase was found to be stable under pressures between 400 MPa and 11.3 GPa. Recently, the α phase was demonstrated to be stable under ambient conditions when the particle sizes were reduced to below 10 nm. However, no other phase has been reported to be stable for silver iodides under ambient conditions. Rock-salt and helix structures have been found to be stable under ambient conditions in this study. The structures have been characterized by elemental mapping, Raman scattering, and high-resolution transmission electron microscopy. The stabilities of these structures were also confirmed by molecular dynamics and density functional theory.

关键词： carbon nanotubes silver iodides rock salt helix ambient conditions

Porous LaFeO3 nanofiber with oxygen vacancies as an efficient electrocatalyst for N2 conversion to NH3 under ambient conditions

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Journal of Energy Chemistry 2020年第11期29卷 402-408页

作者： Chengbo Li Dongwei Ma Shiyong Mou Yongsong Luo Benyuan Ma Siyu Lu Guanwei Cui Quan Li Qian Liu Xuping Sun College of Chemistry and Materials Science Sichuan Normal UniversityChengdu 610068SichuanChina Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054SichuanChina Key Laboratory for Special Functional Materials of Ministry of Education and School of Materials Science and EngineeringHenan UniversityKaifeng 475004HenanChina Green Catalysis Center and College of Chemistry Zhengzhou UniversityZhengzhou 450001HenanChina College of Chemistry Chemical Engineering and Materials ScienceShandong Normal University.Jinan 250014ShandongChina

Electrocatalytic N2 reduction to NH3 under ambient conditions is an eco-friendly and sustainable alternative to the traditional Haber-Bosch process. However, inhibited by the high activation barrier of N2, this process needs efficient electrocatalysts to adsorb and activate the N2, enabling the N2 reduction reaction(NRR). Herein, we report that porous LaFeO3 nanofiber with oxygen vacancies acts as an efficient NRR electrocatalyst with abundant active sites to enhance the adsorption and activation of N2. When tested in 0.1 M HCl, such electrocatalyst achieves a high Faradaic efficiency of 8.77% and a large NH3 yield rate of 18.59 μg h–1 mgcat–1.at-0.55 V versus reversible hydrogen electrode. This catalyst also shows high long-term electrochemical stability and excellent selectivity for NH3 formation. Density functional theory calculations reveal that, by introducing oxygen vacancy on LaFeO3, the subsurface metallic ions are exposed with newly localized electronic states near the Fermi level, which facilitates the adsorption and activation of N2 molecules as well as the subsequent hydrogenation reactions.

关键词： N2 reduction reaction Oxygen vacancies Porous nanofiber ambient conditions Density functional theory

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Oxygen-deficient SnO_(2)nanoparticles with ultrathin carbon shell for efficient electrocatalytic N_(2)reduction

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Green Energy & Environment 2022年第4期7卷 672-679页

作者： Guangkai Li Haeseong Jang Zijian Li Jia Wang Xuqiang Ji Min Gyu Kim Xien Liu Jaephil Cho State Key Laboratory Base of Eco-chemical Engineering College of Chemical EngineeringCollege of Chemistry and Molecular EngineeringQingdaoUniversity of Science and TechnologyQingdao266042China Department of Energy Engineering School of Energy and Chemical EngineeringUlsan National Institute of Science and Technology(UNIST)Ulsan689-798South Korea College of Materials Science and Engineering Qingdao UniversityQingdao266071China Beamline Research Division Pohang Accelerator Laboratory(PAL)Pohang790-784South Korea

For high-efficiency NH_(3)synthesis via ambient-condition electrohydrogenation of inert N_(2),it is pivotal to ingeniously design an active electrocatalyst with multiple features of abundant surfacial deficiency,good conductivity and large surface area.Here,oxygen-deficient SnO_(2)nanoparticles encapsulated by ultrathin carbon layer(d-SnO_(2)@C)are developed by hydrothermal deposition coupled with annealing process,as promising catalysts for ambient electrocatalytic N_(2)reduction.d-SnO_(2)@C exhibits high activity and excellent selectivity for electrocatalytic conversion of N_(2)to NH_(3)in acidic electrolytes,with Faradic efficiency as high as 12.7%at-0.15 V versus the reversible hydrogen electrode(RHE)and large NH_(3)yield rate of 16.68μg h^(-1)mgcat^(-1)at-0.25 V vs.RHE in 0.1 mol L^(-1)HCl.Benefiting from the structural superiority of enhanced charge transfer efficiency and optimized surface states,d-SnO_(2)@C also achieves excellent long-term stability.

关键词： N_(2)reduction reaction NH_(3)synthesis SnO_(2) Electrocatalysts ambient conditions

Research progress in green synthesis of ammonia as hydrogen-storage carrier under‘hydrogen 2.0 economy’

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Clean Energy 2023年第1期7卷 116-131页

作者： Ge Li Ziran Ma Jia Zhao Jiali Zhou Shengpan Peng Yonglong Li Baodong Wang National Institute of Clean-and-Low-Carbon Energy Beijing 102211China Industrial Catalysis Institute of Zhejiang University of Technology Hangzhou 310014ZhejiangChina NICE Europe Research GmbH Stockholmer Platz 170173 StuttgartGermany

Hydrogen energy is characterized by its environmental friendliness,high efficiency,lack of carbon emissions and wide range of applications.However,its transportation and storage are challenges that limit further development of the hydrogen-energy industry.Ammonia is a carbon-free hydrogen-rich carrier.The storage of hydrogen in ammonia has unique advantages of high energy density,easy storage and transportation,reliable safety,a mature industrial foundation and no tail-end carbon emissions.However,industrial ammonia synthesis still heavily relies on the Haber-Bosch process,which accounts for significant energy consumption and greenhouse gas emissions.Therefore,the development of green and sustainable ammonia-synthesis methods is extremely important and urgent.Recently,ammonia-synthesis technologies such as electrocatalysis,photocatalysis,photoelectrocatalysis and biocatalysis have successfully produced ammonia from nitrogen and water,resulting in lower costs.The nitrogen-reduction-reaction conditions of these methods are mild and can be carried out under ambient temperatures and atmospheric pressure with low energy consumptions.Meanwhile,these methods bypass the traditional hydrogen-production section and their routes are simpler.Therefore,these technologies can be used to flexibly integrate renewable energy,including intermittent renewable energy,to achieve distributed ammonia synthesis.These benefits contribute to both global energy and environmental sustainability goals.In this study,the mechanisms of ammonia synthesis under ambient conditions are reviewed and the technical difficulties of various catalysts for ammonia synthesis are summarized.Based on the optimization strategies reported for various catalysts,the high-performing catalysts reported for ammonia synthesis are reviewed and the developmental trend of this field has been forecasted.

关键词： hydrogen 2.0 economy ammonia synthesis catalyst ambient conditions mechanism

A Porous Metal-organic Framework with Ultra-high Acetylene Uptake Capacity under ambient conditions

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A Porous Metal-organic Framework with Ultra-high Acetylene U...

Controllable and large-area growth of ZnO nanosheet arrays under ambient condition as superior anodes for scalable aqueous batteries

中国化学会第九届全国无机化学学术会议

作者： Jiandong Pang Mingyan Wu Caiping Liu Feilong Jiang Maochun Hong State Key Laboratory of Structure Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences University of Chinese Academy of Sciences

Acetylene is a very important chemical feedstock for modern industry.Many widely used polymer products such as polyurethane and polyester plastics are synthesized from acetylene.1 However,the safe storage and transportation of acetylene still remain challenging because of its explosiveness when compressed under pressures over 2 atm at room temperature.2-5 Here we present a porous metal-organic framework([Cu4(tddb)·(H2O)4]n·(solvent)x,abbreviated as FJI-H8),with both suitable pore space and rich open metal sites,for efficient storage of acetylene under ambient conditions.Compared with existing reports,FJI-H8 shows a record-high gravimetric acetylene uptake of 224 cm3(STP)g-1 and the second-highest volumetric uptake of 196cm3(STP)cm-3 at 295 K and 1 atm.Increasing the storage temperature to 308 K has only a small effect on its acetylene storage capacity(00 cm3(STP)g-1).Furthermore,FJI-H8 exhibits an excellent repeatability with only3.8%loss of its acetylene storage capacity after five cycles of adsorption-desorption tests.Grand canonical Monte Carlo simulation reveals that not only open metal sites but also the suitable pore space and geometry play key roles in its remarkable acetylene uptake.

关键词： Porous Metal-organic Framework Acetylene Uptake ambient conditions

来源： cnki会议评论

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Carbon Energy 2023年第12期5卷 241-251页

作者： Dongdong Zhang Yanqing Fu Qiliang Wei Yapeng Zheng Lin Wang Jie Teng Weiyou Yang Institute of Micro/Nano Materials and Devices Ningbo University of TechnologyNingboZhejiangPeople's Republic of China College of Materials Science and Engineering Hunan UniversityChangshaPeople's Republic of China

Two-dimensional(2D)oxides have been the focus of substantial research interest recently,owing to their fascinating physico-chemical properties.However,fabrication of large-area 2D oxide materials in a controlled manner under mild conditions still remains a formidable challenge.Herein,we develop a facile and universal strategy based on the sonochemistry approach for controllable and large-area growth of quasi-aligned single-crystalline ZnO nanosheets on a Zn substrate(Zn@SC-ZnO)under ambient conditions.The obtained ZnO nanosheets possess the desired exclusively exposed(001)facets,which have been confirmed to play a critical role in significantly reducing the activation energy and facilitating the stripping/plating processes of Zn.Accordingly,the constructed Zn@SC-ZnO||Zn@SC-ZnO symmetric cell has very low polarization overpotential down to~20 mV,with limited dendrite growth and side reactions for Zn anodes.The developed Zn@SC-ZnO//MnO_(2)aqueous Zn-ion batteries(ZIBs)show a voltage efficiency of 88.2%under 500 mA g^(-1)at the stage of 50%depth of discharge,which is state of the art for ZIBs reported to date.Furthermore,the as-assembled large-size cell(5 cm×5 cm)delivers an open circuit potential of 1.648 V,and can be robustly operated under a high current of 20 mA,showing excellent potential for future scalable applications.

关键词： ambient conditions aqueous Zn-ion batteries crystal growth nanosheet arrays ZnO

FeOOH quantum dots decorated graphene sheet:An efficient electrocatalyst for ambient N2 reduction

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Nano Research 2020年第1期13卷 209-214页

作者： Xiaojuan Zhu Jinxiu Zhao Lei Ji Tongwei Wu Ting Wang Shuyan Gao Abdulmohsen Ali Alshehri Khalid Ahmed Alzahrani Yonglan Luo Yimo Xiang Baozhan Zheng Xuping Sun Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu610054China Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province College of Chemistry and Chemical EngineeringChina West Normal UniversityNanchong637002China School of Materials Science and Engineering Henan Normal UniversityXinxiang453007China Chemistry Department Faculty of ScienceKing Abdulaziz UniversityP.O.Box 80203Jeddah21589Saudi Arabia No.12 Middle School Chengdu610041China College of Chemistry Sichuan UniversityChengdu610064China

Electrochemical N2 reduction offers a promising alternative to the Haber-Bosch process for sustainable NH3 synthesis at ambient conditions,but it needs efficient catalysts for the N2 reduction reaction(NRR).Here,we report that FeOOH quantum dots decorated graphene sheet acts as a superior catalyst toward enhanced electrocatalytic N2 reduction to NH3 under ambient conditions.In 0.1 M LiClO4,this hybrid attains a large NH3 yield rate and a high Faradaic efficiency of 27.3µg·h^−1·mg−1cat.and 14.6%at−0.4 V vs.reversible hydrogen electrode,respectively,rivalling the current efficiency of all Fe-based NRR electrocatalysts in aqueous media.It also shows strong durability during the electrolytic process.

关键词： FeOOH quantum dots decorated graphene sheet N2 reduction reaction NH3 electrosynthesis ambient conditions