Unraveling the Synergy of Chemical Hydroxylation and the Physical Heterointerface upon Improving the Hydrogen Evolution Kinetics

被引：80

作者：

Liu, Yang ^{[1
,2
]}

Liu, Xinghui ^{[1
,2
]}

Wang, Xiaoshan ^{[3
]}

Ning, Hui ^{[3
]}

Yang, Taehun ^{[1
,2
]}

Yu, Jianmin ^{[1
,2
]}

Kumar, Ashwani ^{[1
,2
]}

Luo, Yongguang ^{[1
,2
]}

Wang, Hongdan ^{[1
,2
]}

Wang, Lingling ^{[1
]}

Lee, Jinsun ^{[1
,2
]}

Jadhav, Amol R. ^{[1
]}

Hu, Han ^{[3
]}

Wu, Mingbo ^{[3
]}

Kim, Min Gyu ^{[4
]}

Lee, Hyoyoung

机构：

[1] Sungkyunkwan Univ, Inst Basic Sci IBS, Ctr Integrated Nanostruct Phys, Suwon 16419, South Korea

[2] Sungkyunkwan Univ, Dept Chem, Suwon 16419, South Korea

[3] China Univ Petr East China, Coll Chem Engn, Inst New Energy, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R China

[4] Pohang Univ Sci & Technol, Pohang Accelerator Lab PAL, Beamline Res Div, Pohang 37673, South Korea

来源：

ACS NANO | 2021年 / 15卷 / 09期

关键词：

transition metal oxides; hydroxylation; water dissociation; heterointerface; hydrogen spillover; improved HER kinetics; ELECTROCATALYTIC ACTIVITY; NI NANOPARTICLES; AC-IMPEDANCE; SURFACE; CU; HYDROXIDE; CATALYSTS; PLATINUM; DENSITY; TRENDS;

D O I：

10.1021/acsnano.1c05324

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Efficient transition metal oxide electrocatalysts for the alkaline hydrogen evolution reaction (HER) have received intensive attention to energy conversion but are limited by their sluggish water dissociation and unfavorable hydrogen migration and coupling. Herein, systematic density functional theory (DFT) predicts that on representative NiO, the hydroxylation (OH-) and heterointerface coupled with metallic Cu can respectively reduce the energy barrier of water dissociation and facilitate hydrogen spillover. Motivated by theoretical predictions, we subtly designed a delicate strategy to realize the electrochemical OH- modification in KOH with moderate concentration (HOM-NiO) and to channel rapid hydrogen spillover at the heterointerface of HOM-NiO and Cu, ensuring an enhanced HER kinetic. This HOM-NiO/Cu is systematically investigated by in situ XAS and electrochemical simulations, verifying its extraordinary merits for HER including the enhanced water dissociation, alleviated oxophilicity that is advantageous for consecutive adsorptions of water, and accelerated hydrogen spillover, thereby exhibiting superb HER activity with 33 and 310 mV overpotentials at the current densities of 10 and 1000 mA cm(-2) in 1.0 M KOH, outperforming the Pt/C. This study might provide a reasonable strategy for the functionalized design of superior electrocatalysts.

引用

页码：15017 / 15026

页数：10

共 51 条

[1] Synergistic effect of nano-Pt and Ni spine for HER in alkaline solution: hydrogen spillover from nano-Pt to Ni spine [J].