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Highly efficient electrocatalytic nitrogen fixation enabled by the bridging effect of Ru in plasmonic nanoparticles

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Nano Research 2023年第1期16卷 360-370页

作者： Hang Yin Jinwu Hu Caihong Fang Yuyang Wang Lixia Ma Nan Zhang Shouren Zhang Ruibin Jiang Jianfang Wang Shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy TechnologySchool of Materials Science and EngineeringShaanxi Normal UniversityXi’an 710119China College of Chemistry and Materials Science The Key Laboratory of Functional Molecular SolidsMinistry of EducationAnhui Laboratory of Molecular-Based MaterialsCenter for Nano Science and TechnologyKey Laboratory of Electrochemical Clean Energy of Anhui Higher Education InstitutesAnhui Normal UniversityWuhu 241000China Henan Provincial Key Laboratory of Nanocomposites and Applications Institute of Nanostructured Functional MaterialsHuanghe Science and Technology CollegeZhengzhou 450006China Department of Physics The Chinese University of Hong KongHong Kong 999077China

Plasmon-generated hot electrons show great potential for driving chemical *** utilization efficiency of hot electrons is highly dependent on the interaction of the electronic states at the interfaces between plasmonic nanoparticles and other materials/*** interaction can produce new hybridized electron states,which permit direct hot-electron transfer,a more efficient transfer ***,Au usually has very weak interaction with most molecules because of its inertness,which makes direct hot-electron transfer ***,the improvement of the hot-electron transfer efficiency from Au to N_(2)is demonstrated by introducing a Ru bridging *** the N_(2)fixation rate and Faradic efficiency(FE)are enhanced by the excitation of *** enhancement of the N_(2)fixation rate is found to arise from plasmon-generated hot *** calculations show that the strong interaction of the Ru electronic states with the N_(2)molecular orbitals produces new hybridized electronic states,and the Ru d electrons also strongly couple with the Au sp *** a bridging role of Ru makes direct hot-electron transfer from Au to N_(2)possible,improving the FE of nitrogen *** findings demonstrate a new approach to increasing the utilization efficiency of plasmonic hot electrons for chemical reactions and will be helpful to the design of plasmonic catalysts in the future.

关键词： electrocatalytic nitrogen fixation Au/Ru electrocatalysts localized surface plasmon resonance electronic state hybridization hot electron

Microfluidic-oriented synthesis of enriched iridium nanodots/carbon architecture for robust electrocatalytic nitrogen fixation

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Green Energy & Environment 2024年第3期9卷 544-555页

作者： Hengyuan Liu Xingjiang Wu Yuhao Geng Xin Li Jianhong Xu The State Key Laboratory of Chemical Engineering Department of Chemical EngineeringTsinghua UniversityBeijing100084China

electrocatalytic nitrogen reduction reaction(NRR)is considered as a promising candidate to achieve ammonia synthesis because of clean electric energy,moderate reaction condition,safe operating process and harmless ***,the chemical inertness of nitrogen and poor activated capacity on catalyst surface usually produce low ammonia yield and faradic ***,the microfluidic technology is proposed to efficiently fabricate enriched iridium nanodots/carbon *** to in-situ co-precipitation reaction and microfluidic manipulation,the iridium nanodots/carbon nanomaterials possess small average size,uniform dispersion,high conductivity and abundant active sites,producing good proton activation and rapid electrons transmission and moderate adsorption/desorption *** a result,the as-prepared iridium nanodots/carbon nanomaterials realize large ammonia yield of 28.73 μg h^(-1) cm^(-2) and faradic efficiency of 9.14%in KOH ***,the high ammonia yield of 11.21 μg h^(-1) cm^(-2) and faradic efficiency of 24.30%are also achieved in H_(2)SO_(4) *** microfluidic method provides a reference for large-scale fabrication of nano-sized catalyst materials,which may accelerate the progress of electrocatalytic NRR in industrialization field.

关键词： Iridium nanodots Carbon Microfluidic technology Efficient synthesis electrocatalytic nitrogen fixation

MXene Quantum Dots/Copper Nanocomposites for Synergistically Enhanced N_(2)Electroreduction

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Energy & Environmental Materials 2023年第1期6卷 192-198页

作者： Yonghua Cheng Xingchuan Li Peng Shen Yali Guo Ke Chu School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070China

electrocatalytic N_(2) reduction reaction(NRR)represents an appealing solution for sustainable ammonia production,whereas exploring high-efficiency NRR catalysts is highly desired but extremely ***,we combine Ti_(3) C_(2)T_(x)-MXene quantum dots(MQDs)with porous Cu nanosheets to design a novel heterostructured MQDs/Cu as an effective and durable NRR ***,MQDs/Cu showed a synergistically enhanced NRR activity with an NH_(3) yield of 78.5 lg h^(-1) mg^(-1)(-0.5 V)and a Faradaic efficiency of 21.3%(-0.4 V),far superior to pure MQDs and Cu,and outperforming the majority of the state-of-the-art NRR *** function theory computations demonstrated that the synergy of MQDs and Cu enabled the creation of interfacial Cu-Ti dimer as dual-active-centers to strongly activate the absorbed N 2 and promote the*N_(2)H formation,consequently resulting in the much reduced energy barriers and greatly enhanced NRR performance.

关键词： density functional theory electrocatalytic nitrogen fixation heterostructure MXene quantum dots

Amorphization activated FeB_(2) porous nanosheets enable efficient electrocatalytic N_(2) fixation

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Journal of Energy Chemistry 2021年第2期30卷 82-89,I0004页

作者： Ke Chu Weicong Gu Qingqing Li Yaping Liu Ye Tian Wuming Liu School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070GansuChina Department of Physics College of ScienceHebei North UniversityZhangjiakou 075000HebeiChina Institute of Physics Chinese Academy of SciencesBeijing 100190China

Designing active,robust and cost-effective catalysts for the nitrogen reduction reaction(NRR) is of paramount significance for sustainable electrochemical NH3 ***-metal diborides(TMB_2)have been recently theoretically predicted to be a new class of potential NRR catalysts,but direct experimental evidence is still ***,we present the first experimental demonstration that amorphous FeB_2 porous nanosheets(a-FeB_2 PNSs) could be a highly efficient NRR catalyst,which exhibited an NH3 yield of 39.8 μg h^(-1) mg^(-1)(-0.3 V) and a Faradaic efficiency of 16.7%(-0.2 V),significantly outperforming their crystalline counterpart and most of existing NRR ***-principle calculations unveiled that the amorphization could induce the upraised d-band center of a-FeB_2 to boost d-2π~* coupling between the active Fe site and ~*N_2 H intermediate,resulting in enhanced ~*N_2 H stabilization and reduced reaction *** study may facilitate the development and understanding of earth-abundant TMB_2-based catalysts for electrocatalytic N_2 fixation.

关键词： electrocatalytic nitrogen fixation Transition-metal diborides Amorphization Density functional theory

Zn nanosheets:An earth-abundant metallic catalyst for efficient electrochemical ammonia synthesis

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Journal of Energy Chemistry 2021年第3期30卷 318-322页

作者： Qingqing Li Jing Wang Yonghua Cheng Ke Chu School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070GansuChina

Ammonia(NH_(3)),a critical raw material for various industrial chemicals,is also recognized as a clean and efficient energy carrier for the future energy economy[1].However,the industrial-scale production of NH_(3) strongly relies on the Haber-Bosch process,which involves massive fuel consumption and enormous greenhouse gas emissions[2].Therefore,there is an urgent need to develop sustainable and energy-saving alternative routes for artificial NH3 production.

关键词： electrocatalytic nitrogen fixation Metallic catalysts Zn nanosheets N2 activation First-principle calculations

Enabling efficient electrocatalytic conversion of N2 to NH3 by Ti3C2 MXene loaded with semi-metallic 1T'-MoS2 nanosheets

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Enabling efficient electrocatalytic conversion of N2 to NH3 ...