Micropore-confined Ru nanoclusters catalyst for efficient pHuniversal hydrogen evolution reaction  

作　　者：Xiaoxiao Huang Ruihu Lu Yaping Cen Dunchao Wang Shao Jin Wenxing Chen Geoffrey I NWaterhouse Ziyun Wang Shubo Tian Xiaoming Sun 

机构地区：[1]State Key Laboratory of Chemical Resource Engineering College of Chemistry,Beijing University of Chemical Technology,Beijing 100029,China [2]School of Chemical Sciences,The University of Auckland,Auckland 1010,New Zealand [3]School of Materials Science and Engineering,Beijing Institute of Technology,Beijing 100081,China

出　　处：《Nano Research》2023年第7期9073-9080,共8页纳米研究（英文版）

基　　金：This work was financially supported by the National Key Research and Development Program of China(Nos.2021YFA1502200 and 2022YFA1504003);the National Natural Science Foundation of China(Nos.21935001 and 22101015);the Fundamental Research Funds of Beijing University of Chemical Technology(Nos.buctrc202107 and buctrc202212);The computational study was supported by the Marsden Fund Council(No.21-UOA-237)from Government funding,managed by Royal Society Te Apārangi and Catalyst:Seeding Grant(22-UOA-031-CSG)provided by the New Zealand Ministry of Business,Innovation and Employment and administered by the Royal Society Te Apārangi.Z.Y.W.and R.H.L.wish to acknowledge the use of New Zealand eScience Infrastructure(NeSI)high performance computing facilities,consulting support,and/or training services as part of this research.GINW acknowledges funding support from the Royal Society Te Apārangi(for the award of James Cook Research Fellowship).

摘　　要：Pt-based catalysts are used commercially for the hydrogen evolution reaction(HER),even though the low earth abundance and high cost of platinum hinder scale-up applications.Ru metal is a promising alternative catalyst for HER owing to its lower cost but similar metal-hydrogen bond strength to Pt.However,designing an efficient and robust Ru-based electrocatalyst for pHuniversal HER is challenging.Herein,we successfully synthesized N-doped carbon(NC)supported ruthenium catalysts with different Ru sizes(single-atoms,nanoclusters and nanoparticles),and then systematically evaluated their performance for HER.Among these catalysts,the Ru nanocluster catalyst(Ru NCs/NC)displayed optimal catalytic performance with overpotentials of only 14,30,and 32 mV(at 10 mA·cm^(-2))in 1 M KOH,1 M phosphate buffer saline(PBS),and 0.5 M H_(2)SO_(4),respectively.The corresponding mass activities were 32.2,12.1 and 8.1 times higher than those of 20 wt.%Pt/C,and also much better than those of the Ru single-atoms(Ru SAs/NC)and Ru nanoparticle(Ru NPs/NC)catalysts,at an overpotential of 100 mV under alkaline,neutral and acidic conditions,respectively.Density functional theory(DFT)calculations revealed that the outstanding HER performance of the Ru NCs/NC catalyst resulted from a strong interaction between the Ru nanoclusters and the N-doped carbon support,which downshifted the d-band center and thus weakened the*H adsorption ability of Ru sites.

关 键 词：Ru nanoclusters Ru single atoms Ru nanoparticles hydrogen evolution reaction 

分 类 号：O64[理学—物理化学]