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研究钼锚定氮掺杂碳中用于碱性析氧反应的活性位点。

Investigating the active sites in molybdenum anchored nitrogen-doped carbon for alkaline oxygen evolution reaction.

作者信息

Wang Yuan, Dong Rui, Tan Pengfei, Liu Hongqin, Liao Hanxiao, Jiang Min, Liu Yong, Yang Lu, Pan Jun

机构信息

State Key Laboratory for Powder Metallurgy, Central South University, Changsha 410083, PR China.

State Key Laboratory for Powder Metallurgy, Central South University, Changsha 410083, PR China.

出版信息

J Colloid Interface Sci. 2022 Mar;609:617-626. doi: 10.1016/j.jcis.2021.11.058. Epub 2021 Nov 15.

Abstract

Developing durable and efficient non-precious-metal based catalysts for oxygen evolution reaction (OER) is highly desirable in the field of electrocatalysis. In this work, a series of novel Mo anchored N-doped carbon catalysts (denoted as Mo/NC-T) were prepared starting from the zeolitic imidazolate framework 8 (ZIF-8) precursor. Firstly, Mo doped ZIF-8 precursor (Mo/ZIF-8) with a regular polyhedron structure was formed through a simple ion-exchange method process between molybdenum pentachloride (MoCl) and ZIF-8. Afterward, Mo/ZIF-8 was converted to Mo/NC-T through a two-step calcination process in nitrogen (N) and ammonia (NH). The as-synthesized Mo/NC-T samples exhibited superior electrocatalytic OER properties. The optimal sample at 650 °C (Mo/NC-650) presented a low overpotential of 320 mV at 10 mA cm, a Tafel slope of 71 mV dec, and an outstanding long-term stability for 30 h in 1 M KOH solution. The remarkable OER activity of Mo/NC-T could be ascribed to the structural stability of carbon matrix and the synergistic effect between Mo (derived from Mo-C bonds) and pyridinic N. This work provides a novel perspective on the roles of Mo species in the N-doped carbon electrocatalysts for OER.

摘要

开发用于析氧反应(OER)的耐用且高效的非贵金属基催化剂在电催化领域非常必要。在这项工作中,从沸石咪唑酯骨架8(ZIF-8)前驱体出发制备了一系列新型的钼锚定氮掺杂碳催化剂(记为Mo/NC-T)。首先,通过五氯化钼(MoCl)与ZIF-8之间简单的离子交换法形成具有规则多面体结构的钼掺杂ZIF-8前驱体(Mo/ZIF-8)。之后,Mo/ZIF-8通过在氮气(N)和氨气(NH)中进行两步煅烧过程转化为Mo/NC-T。所合成的Mo/NC-T样品表现出优异的电催化OER性能。在650°C下制备的最佳样品(Mo/NC-650)在10 mA cm时具有320 mV的低过电位、71 mV dec的塔菲尔斜率,并且在1 M KOH溶液中具有30小时出色的长期稳定性。Mo/NC-T卓越的OER活性可归因于碳基体的结构稳定性以及Mo(源自Mo-C键)与吡啶氮之间的协同效应。这项工作为钼物种在用于OER的氮掺杂碳电催化剂中的作用提供了新的视角。

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