Highly Active and Durable Single-Atom Tungsten-Doped NiS0.5Se0.5 Nanosheet @ NiS0.5Se0.5 Nanorod Heterostructures for Water Splitting

被引：287

作者：

Wang, Yang ^{[1
,2
]}

Li, Xiaopeng ^{[1
]}

Zhang, Mengmeng ^{[1
,3
]}

Zhang, Jinfeng ^{[1
]}

Chen, Zelin ^{[2
]}

Zheng, Xuerong ^{[1
,2
]}

Tian, Zhangliu ^{[4
]}

Zhao, Naiqin ^{[1
]}

Han, Xiaopeng ^{[1
]}

Zaghib, Karim ^{[5
]}

Wang, Yuesheng ^{[5
]}

Deng, Yida ^{[1
,2
]}

Hu, Wenbin ^{[1
,6
]}

机构：

[1] Tianjin Univ, Key Lab Adv Ceram & Machining Technol, Tianjin Key Lab Composite & Funct Mat, Sch Mat Sci & Engn,Minist Educ, Tianjin 300350, Peoples R China

[2] Hainan Univ, State Key Lab Marine Resource Utilizat South Chin, Sch Mat Sci & Engn, Haikou 570228, Hainan, Peoples R China

[3] Tiangong Univ, Sch Mat Sci & Engn, Tianjin 300387, Peoples R China

[4] Natl Univ Singapore, Dept Chem, 3 Sci Dr 3, Singapore 117543, Singapore

[5] Hydro Quebec, Ctr Excellence Transportat Electrificat & Energy, 1800 Blvd Lionel Boulet, Varennes, PQ J3X 1S1, Canada

[6] Tianjin Univ, Joint Sch Natl Univ Singapore & Tianjin Univ, Int Campus, Fuzhou 350207, Peoples R China

来源：

ADVANCED MATERIALS | 2022年 / 34卷 / 13期

基金：

中国国家自然科学基金;

关键词：

delocalization of spin states; electrocatalysts; homojunctions; nanorods; nanosheets; single-atom catalysts; water splitting; MOS2 ULTRATHIN NANOSHEETS; HYDROGEN-EVOLUTION; EDGE SITES; BIFUNCTIONAL ELECTROCATALYSTS; EFFICIENT; CATALYST; NANOPARTICLES; SURFACE; CARBON; IDENTIFICATION;

D O I：

10.1002/adma.202107053

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Developing robust and highly active non-precious electrocatalysts for the hydrogen/oxygen evolution reaction (HER/OER) is crucial for the industrialization of hydrogen energy. In this study, a highly active and durable single-atom W-doped NiS0.5Se0.5 nanosheet @ NiS0.5Se0.5 nanorod heterostructure (W-NiS0.5Se0.5) electrocatalyst is prepared. W-NiS0.5Se0.5 exhibits excellent catalytic activity for the HER and OER with ultralow overpotentials (39 and 106 mV for the HER and 171 and 239 mV for the OER at 10 and 100 mA cm(-2), respectively) and excellent long-term durability (500 h), outperforming commercial precious-metal catalysts and many other previously reported transition-metal-based compounds (TMCs). The introduction of single-atom W delocalizes the spin state of Ni, which results in an increase in the Ni d-electron density. This causes the optimization of the adsorption/desorption process of H and a significant reduction in the adsorption free energy of the rate-determining step (O* -> OOH*), thus accelerating the thermodynamics and kinetics of the HER and OER. This work provides a rational feasible strategy to design single-atom catalysts for water splitting and to develop advanced TMC electrocatalysts by regulating delocalized spin states.

引用

页数：10

共 61 条

[1]

Bai S., 2014, ANGEW CHEM-GER EDIT, V126, P12320

[2] Identification of single-atom active sites in carbon-based cobalt catalysts during electrocatalytic hydrogen evolution [J].