Mo2C的原位合成及增强Co基催化剂氨硼烷水解产氢性能

doi:10.16085/j.issn.1000-6613.2022-2286

摘要/Abstract

摘要：

为了研究Mo₂C与Co之间的协同作用对催化氨硼烷水解制氢的影响，采用分步浸渍法制备了Co-30Mo₂C/CNTs复合纳米材料。采用X射线衍射、扫描电子显微镜和X射线光电子能谱对催化剂进行表征，并考察了其催化氨硼烷水解制氢性能。结果表明，实验方法成功合成Co-30Mo₂C/CNTs，Co和Mo₂C可以较均匀分散在CNTs周围，且Mo₂C可以局部生长成棒状结构，对团聚成块状的CNTs起支撑作用，使催化剂可以具有更多空隙，暴露更多活性位点。对Co-30Mo₂C/CNTs、30Mo₂C/CNTs和10Co/CNTs中的Co、Mo元素结合能进行分析，发现存在部分电子转移，影响并改善了Co-30Mo₂C/CNTs的催化活性。Co-30Mo₂C/CNTs催化氨硼烷水解产氢速率最高，可达11866，这优异的催化活性归结于Co和Mo₂C之间的协同作用，Mo₂C的添加增强了对H₂O分子的活化。经过五圈稳定性测试后，活性依然可以保留75%，这对非贵金属催化剂的可回收投入使用具有一定的研究意义。

关键词: 氨硼烷, 制氢, 催化剂, 催化作用, 钴, 碳化钼, 催化剂载体

Abstract:

In order to study the synergistic effect between Mo₂C and Co on the catalytic hydrolysis of ammonia borane to hydrogen, Co-30Mo₂C/CNTs nanomaterial was prepared by a step impregnation method. The synthesized catalysts were characterized by X-ray diffraction, scanning electron microscopy and X-ray photoelectron spectroscopy, and their catalytic performance of ammonia borane hydrolysis was tested. The results showed that Co-30Mo₂C/CNTs was successfully synthesized, Co and Mo₂C were evenly dispersed around CNTs. Mo₂C grew into rod-shaped structures locally, which could play a supporting role for the agglomerated CNTs, and hence the catalyst possessed more voids and exposed more active sites. The binding energies of Co and Mo in Co-30Mo₂C/CNTs, 30Mo₂C/CNTs and 10Co/CNTs were analyzed. It was found that there was partial electron transfer, which improved the catalytic activity of Co-30Mo₂C/CNTs. The hydrogen production rate of Co-30Mo₂C/CNTs was the highest, reaching 11866. This excellent catalytic activity can be attributed to the synergistic effect between Co and Mo₂C. The addition of Mo₂C enhanced the activation of H₂O molecules. After five cycles of stability test, 75% of the activity were retained, which is of significance for the recyclability of non-precious metal catalysts.

Key words: ammonia borane, hydrogen production, catalyst, catalysis, Co, Mo₂C, catalyst support

中图分类号:

TQ426.8

段继转, 刘宪云. Mo₂C的原位合成及增强Co基催化剂氨硼烷水解产氢性能[J]. 化工进展, 2023, 42(11): 5730-5737.

DUAN Jizhuan, LIU Xianyun. In-situ synthesis of Mo₂C and enhancement of Co based catalyst for hydrogen production from ammonia borane hydrolysis[J]. Chemical Industry and Engineering Progress, 2023, 42(11): 5730-5737.

图/表 6

图1 不同催化剂的XRD图谱

图2 CNTs和10Co/CNTs的SEM图、EDS谱图

图3 Co-30Mo2C/CNTs的SEM图和EDS谱图

图4 30Mo2C/CNTs、10Co/CNTs和Co-30Mo2C/CNTs的XPS光谱

图5 不同催化剂的AB水解产氢活性曲线和产氢速率

图6 Co-30Mo2C/CNTs在不同温度下的活性曲线、产氢速率、稳定性测试和不同NaOH浓度下的催化活性

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Mo₂C的原位合成及增强Co基催化剂氨硼烷水解产氢性能

In-situ synthesis of Mo₂C and enhancement of Co based catalyst for hydrogen production from ammonia borane hydrolysis

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