High valence state of Ni and Mo synergism in NiS2-MoS2 hetero-nanorods catalyst with layered surface structure for urea electrocatalysis
High valence state of Ni and Mo synergism in NiS2-MoS2 hetero-nanorods catalyst with layered surface structure for urea electrocatalysis
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DOI：
10.1016/j.jechem.2021.08.042
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发表时间：
2021-09-21
影响因子：
13.1
通讯作者：
Feng, Ligang
中科院分区：
文献类型：
--
作者：
Wang, Shuli;Zhao, Linyu;Feng, Ligang
高价态物种在能量相关的电化学氧化反应中具有重要意义。本文论证了Mo6+在具有粗糙层状结构的NiS2-MoS2杂化纳米棒粉末催化剂中诱导Ni3+生成的高活性状态及其高效的协同作用，作为尿素辅助水电解的概念验证。这种催化剂可以由NiMoO4纳米棒硫化而来，可以实现单个金属硫化物在纳米尺度上以一定的区域尺寸充分混合，从而产生大量的活性中心和纳米界面。光谱研究和显微分析表明，与纯相相比，杂化纳米棒中Mo6+和Ni3+的生成价态较高，1T MoS2的导电相增加；纳米界面的形成和纳米棒表面的层状粗糙纳米片使其具有较高的电化学比表面积和活性位暴露。它们对尿素氧化表现出比纯相高得多的催化性能，包括高催化活性、稳定性、电荷转移能力，以及由于高价金属形成更活跃的Ni3+物种和电子协同作用而导致的催化动力学。1T MoS2转化为Mo6+，稳定性试验后Mo6+和Ni3+含量增加，说明它们对催化反应有一定的参与和协同作用。本工作为基于高价态协同效应的多相催化剂在电催化中的协同效应提供了新的理解。(C)2021科学出版社和中国科学院大连化学物理研究所。由Elsevier B.V.和科学出版社出版。版权所有。
High valence state species are significant in the energy-relevant electrochemical oxidation reactions. Herein, the high active state of Ni3+ formation induced by Mo6+ and their efficient synergism in NiS2-MoS2 hetero-nanorods powder catalyst with the rough layered structure are demonstrated, as proof of concept, for the urea-assisted water electrolysis. This catalyst can be derived from the sulfidation of NiMoO4 nanorods that can realize individual metal sulfides sufficiently mixing at a domain size in the nanoscale which creates lots of active sites and nanointerfaces. The high valence state of Mo6+ and Ni3+ formation and increased conductive phase of 1 T MoS2 in the hetero-nanorods compared to the counterpart pure phases are revealed by spectral study and microscopic analysis; high electrochemical surface area and active site exposure are found due to the nano-interface formation and layered rough nanosheets over the surface of nanorods. They show much higher catalytic performance than their pure phases for urea oxidation, including high catalytic activity, stability, charge transfer ability and catalytic kinetics resulting from more active Ni3+ species formation and electronic synergism of high valence metals. Transformation of 1 T MoS2 to Mo6+ and increased amount of Mo6+ and Ni3+ after stability test indicate their involvement and synergism for the catalysis reaction. The current work offers a novel understanding of the synergistic effect based on the high valence state synergism for heterogeneous catalysts in electrocatalysis. (C) 2021 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.