Constructing Co@TiO<sub>2</sub> Nanoarray Heterostructure with Schottky Contact for Selective Electrocatalytic Nitrate Reduction to Ammonia

Xiaoya Fan(University of Electronic Science and Technology of China), Donglin Zhao(University of Electronic Science and Technology of China), Zhiqin Deng(University of Electronic Science and Technology of China), Longcheng Zhang(University of Electronic Science and Technology of China), Jun Li(University of Electronic Science and Technology of China), Zerong Li(University of Electronic Science and Technology of China), Shengjun Sun(Shandong Normal University), Yongsong Luo(University of Electronic Science and Technology of China), Dongdong Zheng(University of Electronic Science and Technology of China), Yan Wang(University of Electronic Science and Technology of China), Binwu Ying(University of Electronic Science and Technology of China), Jing Zhang(Chengdu University), Abdulmohsen Ali Alshehri(King Abdulaziz University), Yuxiao Lin(Jiangsu Normal University), Chengwu Tang(Huzhou University), Xuping Sun(University of Electronic Science and Technology of China), Yinyuan Zheng(Huzhou University)
Small
January 30, 2023
10.1002/smll.202208036
Cited by 156

Abstract

Abstract Electrochemical nitrate (NO 3 − ) reduction reaction (NO 3 − RR) is a potential sustainable route for large‐scale ambient ammonia (NH 3 ) synthesis and regulating the nitrogen cycle. However, as this reaction involves multi‐electron transfer steps, it urgently needs efficient electrocatalysts on promoting NH 3 selectivity. Herein, a rational design of Co nanoparticles anchored on TiO 2 nanobelt array on titanium plate (Co@TiO 2 /TP) is presented as a high‐efficiency electrocatalyst for NO 3 − RR. Density theory calculations demonstrate that the constructed Schottky heterostructures coupling metallic Co with semiconductor TiO 2 develop a built‐in electric field, which can accelerate the rate determining step and facilitate NO 3 − adsorption, ensuring the selective conversion to NH 3 . Expectantly, the Co@TiO 2 /TP electrocatalyst attains an excellent Faradaic efficiency of 96.7% and a high NH 3 yield of 800.0 µmol h −1 cm −2 under neutral solution. More importantly, Co@TiO 2 /TP heterostructure catalyst also presents a remarkable stability in 50‐h electrolysis test.

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