文献类型：期刊文献

英文题名：Understanding hydrogen electrocatalysis by probing the hydrogen-bond network of water at the electrified Pt-solution interface

作者：Sun, Qiang[1];Oliveira, Nicholas J.[2];Kwon, Soonho[3,4];Tyukhtenko, Sergiy[5,6,7,8];Guo, Jason J.[1,9];Myrthil, Nathalie[1];Lopez, Steven A.[1];Kendrick, Ian[1];Mukerjee, Sanjeev[1];Ma, Lu[10];Ehrlich, Steven N.[10];Li, Jingkun[11];Goddard, William A., III[3,4];Yan, Yushan[2];Jia, Qingying[1]

机构：[1]Northeastern Univ, Dept Chem & Chem Biol, Boston, MA 02118 USA;[2]Univ Delaware, Ctr Clean Hydrogen, Dept Chem & Biomol Engn, Newark, DE 19716 USA;[3]CALTECH, Liquid Sunlight Alliance LiSA, Pasadena, CA 91125 USA;[4]CALTECH, Mat & Proc Simulat Ctr MSC, Pasadena, CA USA;[5]Northeastern Univ, Ctr Drug Discovery, Boston, MA USA;[6]Northeastern Univ, Dept Pharmaceut Sci, Boston, MA USA;[7]Northeastern Univ, Dept Chem, Boston, MA USA;[8]Northeastern Univ, Dept Chem Biol, Boston, MA USA;[9]Northeastern Univ, Barnett Inst Chem & Biol Anal, Boston, MA USA;[10]Brookhaven Natl Lab, Natl Synchrotron Light Source 2, Upton, NY USA;[11]East China Univ Sci & Technol, Sch Chem & Mol Engn, Shanghai, Peoples R China

年份：2023

卷号：8

期号：8

起止页码：859

外文期刊名：NATURE ENERGY

收录：;EI(收录号：20232814366810);WOS:【SCI-EXPANDED(收录号:WOS:001023405800006)】；

基金：This work was supported by the Office of Naval Research (ONR) grant N000141712608 (Q.J.). This research used beamline 7-BM (QAS) of the National Synchrotron Light Source II, a US Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory Contract DE-SC0012704. Beamline operations were supported in part by the Synchrotron Catalysis Consortium Grant DE-SC0012335. W.A.G. acknowledges support by the Liquid Sunlight Alliance, which is supported by the US DOE, Office of Science, Office of Basic Energy Sciences, Fuels from Sunlight Hub under award number DE-SC0021266. This work used the Extreme Science and Engineering Discovery Environment (XSEDE) for AIMD simulation, which is supported by the NSF grant number ACI-1548562. S.K. acknowledges support from the Resnick Sustainability Institute at Caltech.

语种：英文

外文关键词：Electrocatalysis - Electrodes - Hydrogen bonds - Ion exchange membranes

摘要：Hydrogen evolution and oxidation on platinum surfaces are central reactions in electrochemical devices. Sun et al. show that they can be promoted by introduction of the organic molecules, N-methylimidazoles, and explore the underlying phenomena at play through in situ spectroscopy and computation. Rational construction of the electrode-solution interface where electrochemical processes occur is of paramount importance in electrochemistry. Efforts to gain better control and understanding of the interface have been hindered by lack of probing methods. Here we show that the hydrogen evolution and oxidation reactions (HER/HOR) catalysed by platinum in base can be promoted by introduction of N-methylimidazoles at the platinum-water interface. In situ spectroscopic characterization together with simulations indicate that the N-methylimidazoles facilitate diffusion of hydroxides across the interface by holding the second layer of water close to platinum surfaces, thereby promoting the HER/HOR. We thus propose that the HER/HOR kinetics of platinum in acid and base is governed by diffusion of protons and hydroxides, respectively, through the hydrogen-bond network of interfacial water by the Grotthuss mechanism. Moreover, we demonstrate a 40% performance improvement of an anion exchange membrane electrolyser by adding 1,2-dimethylimidazole into the alkali fed into its platinum cathode.