Bimetallic PdFe<sub>3</sub> Nano-Alloy with Tunable Electron Configuration for Boosting Electrochemical Nitrogen Fixation

doi:10.1002/aenm.202303558

IMR OpenIR

	Bimetallic PdFe₃ Nano-Alloy with Tunable Electron Configuration for Boosting Electrochemical Nitrogen Fixation
	Mu, Jianjia 1; Zhao, Zhiwei 2; Gao, Xuan-Wen 1; Liu, Zhao-Meng 1; Luo, Wen-Bin 1; Sun, Zhenhua 3; Gu, Qin-Fen 4; Li, Feng 3
通讯作者	Luo, Wen-Bin(luowenbin@smm.neu.edu.cn) ; Li, Feng(fli@imr.ac.cn)
	2023-12-15
发表期刊	ADVANCED ENERGY MATERIALS
ISSN	1614-6832
页码	10
摘要	Electrocatalyst plays animportant role in electrochemical ammonia synthesis by determining the nitrogen reduction reaction pathway. Featuring the inherent half-filled 3d orbitals, ion-based alloy electrocatalysts have been attracting much more attention owing to the controllable driving force to adsorb and activate N equivalent to N bonds. Besides supplying unoccupied d-orbital to accommodate lone-pair electrons to facilitate nitrogen adsorption, donating d-orbital electrons to nitrogen antibonding orbitals to dissociate N equivalent to N bond is demandedas well. By palladium (Pd) to synthesize PdFe3 nano-alloy, numerous Fe 3d orbitals can be reconstructed via charge polarization between Fe and Pd, simultaneously lowering corresponding work functions. Meanwhile, the positively charged Fesites in PdFe3 can strengthen suppress the proton adsorption by electrostatic repulsion. A considerably optimized ammonia production rate of 29.07 mu g h(-1) mg(cat).(-1) and Faradic efficiency of 22.8% are accomplished at a low overpotential of -0.2 V vs. RHE. Density functional theory combined with in-situ ATR-FTIR results confirmthe electrocatalytic nitrogen reduction follows the associative distalmechanism and the electron-deficient Fe induced through Pd facilitates significantly lowering the first-step-protonation energy barrier of only 0.07 eV (N-2+ H ->*NNH).
关键词	electrocatalyst electrochemical nitrogen fixation electronic configuration PdFe3 nano-alloy
资助者	National Natural Science Foundation of China ; Liaoning Revitalization Talents Program
DOI	10.1002/aenm.202303558
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China ; Liaoning Revitalization Talents Program[XLYC2007155] ; [52272194]
WOS研究方向	Chemistry ; Energy & Fuels ; Materials Science ; Physics
WOS类目	Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter
WOS记录号	WOS:001127270900001
出版者	WILEY-V C H VERLAG GMBH
引用统计	被引频次：39[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/182855
专题	中国科学院金属研究所
通讯作者	Luo, Wen-Bin; Li, Feng
作者单位	1.Northeastern Univ, Inst Energy Electrochem & Urban Mines Met, Sch Met, Shenyang 110819, Liaoning, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Peoples R China 3.Chinese Acad Sci, Inst Met Res, Shenyang 110819, Liaoning, Peoples R China 4.Australian Synchrotron ANSTO, 800 Blackburn Rd, Clayton, Vic 3168, Australia
推荐引用方式 GB/T 7714	Mu, Jianjia,Zhao, Zhiwei,Gao, Xuan-Wen,et al. Bimetallic PdFe₃ Nano-Alloy with Tunable Electron Configuration for Boosting Electrochemical Nitrogen Fixation[J]. ADVANCED ENERGY MATERIALS,2023:10.
APA	Mu, Jianjia.,Zhao, Zhiwei.,Gao, Xuan-Wen.,Liu, Zhao-Meng.,Luo, Wen-Bin.,...&Li, Feng.(2023).Bimetallic PdFe₃ Nano-Alloy with Tunable Electron Configuration for Boosting Electrochemical Nitrogen Fixation.ADVANCED ENERGY MATERIALS,10.
MLA	Mu, Jianjia,et al."Bimetallic PdFe₃ Nano-Alloy with Tunable Electron Configuration for Boosting Electrochemical Nitrogen Fixation".ADVANCED ENERGY MATERIALS (2023):10.