Oxygen Vacancies and Interface Engineering on Amorphous/Crystalline CrOx-Ni3N Heterostructures toward High-Durability and Kinetically Accelerated Water Splitting

Yang，Mingyang1,2; Zhao，Mengxuan1; Yuan，Ji1; Luo，Junxuan1; Zhang，Junjun3; Lu，Zhouguang3; Chen，Dazhu1; Fu，Xianzhu1; Wang，Lei1; Liu，Chen1

2022

10.1002/smll.202106554

Small   影响因子和分区

1613-6810

1613-6829

Manipulating catalytic active sites and reaction kinetics in alkaline media is crucial for rationally designing mighty water-splitting electrocatalysts with high efficiency. Herein, the coupling between oxygen vacancies and interface engineering is highlighted to fabricate a novel amorphous/crystalline CrO-NiN heterostructure grown on Ni foam for accelerating the alkaline hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Density functional theory (DFT) calculations reveal that the electron transfer from amorphous CrO to NiN at the interfaces, and the optimized Gibbs free energies of HO dissociation (ΔG) and H adsorption (ΔG) in the amorphous/crystalline CrO-NiN heterostructure are conducive to the superior and stable HER activity. Experimental data confirm that numerous oxygen vacancies and amorphous/crystalline interfaces in the CrO-NiN catalysts are favorable for abundant accessible active sites and enhanced intrinsic activity, resulting in excellent catalytic performances for HER and OER. Additionally, the in situ reconstruction of CrO-NiN into highly active NiN/Ni(OH) is responsible for the optimized OER performance in a long-term stability test. Eventually, an alkaline electrolyzer using CrO-NiN as both cathode and anode has a low cell voltage of 1.53 V at 10 mA cm, together with extraordinary durability for 500 h, revealing its potential in industrial applications.

alkaline water splitting amorphous/crystalline CrO x-Ni 3N density functional theory interface engineering oxygen vacancy structure reconstruction

SCI ; EI

英语

ESI高被引

其他

WOS:000754186800001

20220711643661

Catalyst activity ; Chromium compounds ; Design for testability ; Durability ; Electrocatalysts ; Electrodes ; Nickel compounds ; Oxygen vacancies ; Reaction kinetics

Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4 ; Crystalline Solids:933.1

2-s2.0-85124510828

Scopus

1.Shenzhen University,Guangdong Research Center for Interfacial Engineering of Functional Materials,Shenzhen Key Laboratory of Polymer Science and Technology,College of Materials Science and Engineering,Shenzhen,518060,China
2.Shenzhen University,Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province,College of Optoelectronic Engineering,Shenzhen,518060,China
3.Southern University of Science and Technology,Guangdong Provincial Key Laboratory of Energy Materials for Electric Power,Department of Materials Science and Engineering,Shenzhen,518055,China

Yang，Mingyang,Zhao，Mengxuan,Yuan，Ji,et al. Oxygen Vacancies and Interface Engineering on Amorphous/Crystalline CrOx-Ni3N Heterostructures toward High-Durability and Kinetically Accelerated Water Splitting[J]. Small,2022,18.

Yang，Mingyang.,Zhao，Mengxuan.,Yuan，Ji.,Luo，Junxuan.,Zhang，Junjun.,...&Liu，Chen.(2022).Oxygen Vacancies and Interface Engineering on Amorphous/Crystalline CrOx-Ni3N Heterostructures toward High-Durability and Kinetically Accelerated Water Splitting.Small,18.

Yang，Mingyang,et al."Oxygen Vacancies and Interface Engineering on Amorphous/Crystalline CrOx-Ni3N Heterostructures toward High-Durability and Kinetically Accelerated Water Splitting".Small 18(2022).