Du Yufei, Zhang Yichu, Pu Xunchi, Fu Xiaoying, Li Xuan, Bai Linqin, Chen Yongjun, Qian Jin
School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xi'an, PR China.
State Key Laboratory of Hydraulics and Mountain River Engineering, Sichuan University, Chengdu, China.
Chemosphere. 2023 Jan;312(Pt 1):137203. doi: 10.1016/j.chemosphere.2022.137203. Epub 2022 Nov 11.
To boost the oxygen evolution reaction (OER) and methanol oxidation reaction (MOR) of pristine NiFe-layered double hydroxides (LDH), the NiFe-LDH/Mo-doped graphitic carbon nitride (NiFe-LDH/MoCN) heterojunction was synthesized herein through hydrothermal method. The establishment of built-in electric field in NiFe-LDH/MoCN heterojunction enhanced the electrochemical oxidation activities towards both seawater splitting and methanol oxidation, via the improving electrocatalyst surface wettability and conductivity. Almost 10-fold enhancement of turnover frequency (TOF) and electrochemical active surface area (ECSA) than pure NiFe-LDH implied more active sites to participate in catalytic reactions via Mo doping and the formation of heterostructure. Moreover, the local charge redistribution demonstrated in the NiFe-LDH/MoCN interface region may favor the adsorption of methanol and OH in the seawater. The present work may expound the strong coupling interaction and the establishment of built-in electric field in the interface between NiFe-LDH and semiconductor to enhance both methanol oxidation and seawater oxidation for NiFe-LDH.
为了提高原始镍铁层状双氢氧化物（LDH）的析氧反应（OER）和甲醇氧化反应（MOR），本文通过水热法合成了镍铁层状双氢氧化物/钼掺杂石墨相氮化碳（NiFe-LDH/MoCN）异质结。NiFe-LDH/MoCN异质结中内建电场的建立，通过改善电催化剂表面润湿性和导电性，增强了对海水分解和甲醇氧化的电化学氧化活性。与纯NiFe-LDH相比，周转频率（TOF）和电化学活性表面积（ECSA）提高了近10倍，这意味着通过钼掺杂和异质结构的形成，有更多的活性位点参与催化反应。此外，NiFe-LDH/MoCN界面区域显示的局部电荷重新分布可能有利于海水中甲醇和OH的吸附。本工作可能阐明了NiFe-LDH与半导体界面之间的强耦合相互作用和内建电场的建立，以增强NiFe-LDH的甲醇氧化和海水氧化性能。
