洁净煤技术2024,Vol.30Issue(1) :173-179.DOI:10.13226/j.issn.1006-6772.KD23091801

H2O2刻蚀MoS2纳米片增强CO2催化加氢性能

Enhanced CO2 catalytic hydrogenation performance by H2O2-etched MoS2 nanosheets

周维 赵世熙 谢欣雨 陆诗建 倪中海 杨菲菲
洁净煤技术2024,Vol.30Issue(1) :173-179.DOI:10.13226/j.issn.1006-6772.KD23091801

H2O2刻蚀MoS2纳米片增强CO2催化加氢性能

Enhanced CO2 catalytic hydrogenation performance by H2O2-etched MoS2 nanosheets

周维 1赵世熙 2谢欣雨 1陆诗建 1倪中海 1杨菲菲1
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作者信息

  • 1. 中国矿业大学 化工学院,江苏 徐州 221116
  • 2. 中国核电工程有限公司 北京 100840
  • 折叠

摘要

CO2催化加氢制备高附加值化学品是缓解温室效应,实现人类社会可持续发展的关键技术之一.二维MoS2材料由于其特殊的层状结构和表面丰富可调的S缺陷位,在CO2活化与转化中被广泛关注,将MoS2 催化剂用于CO2 加氢的关键在于表面S空位的构建.为开发高效构建S 空位工艺,以MoS2纳米片为基础,利用H2O2刻蚀法在其表面引入S空位,对比了H2O2刻蚀前后CO2在常压和高压下的反应性能.研究表明,H2O2刻蚀能显著提升S空位含量,且不会改变MoS2的晶相结构,也未影响S空位的化学性质,从而明显提升CO2催化加氢的转化率,但不影响产物分布.在常压条件下,S空位主要催化CO2解离加氢为CO,选择性达 96%以上;而在高压(5 MPa)低温(180℃)条件下能以较高的选择性(79%)催化CO2加氢为甲醇,升高反应温度会提升CO2转化率,但甲醇的选择性会显著降低,同时伴随甲烷的生成.本研究提供了一种简便高效的构造S空位的制备工艺,为MoS2催化剂的工业化应用提供一定的理论和技术支撑.

Abstract

Catalytic hydrogenation of CO2 to valuable chemicals is one of the key technologies to relieve global warming and promote the sustainable development of human society.Two-dimensional MoS2 materials have emerged as promising catalysts for CO2 activation and conversion due to their unique layered structure and adjustable S vacancies sites,which is the key active center for CO2 hydrogenation.In order to develop an efficient process for S vacancy creation,building S vacancies on MoS2 nanosheet were used as the basis for introdu-cing S vacancies on the surface using H2O2 etching method,and the reaction properties of CO2 at atmosphere and high pressure before and after H2O2 etching were compared.The results show that H2O2 etching can significantly enhance the content of S vacancies without chan-ging the crystal structure of MoS2 or affecting the chemical properties of S vacancy sites,which significantly enhances the conversion rate of CO2 catalytic hydrogenation without affecting the product distribution.Specifically,the S vacancies catalyze CO2 dissociation to produce CO at atmosphere pressure with selectivity higher than 96%,whereas they are able to catalyze the hydrogenation of CO2 to the methanol at high pressure of 5 MPa and 180℃ with high selectivity(79%).Increasing the reaction temperature improves the CO2 conversion,but the selectivity of methanol will be signifi-cantly reduced,accompanied by the generation of methane.Briefly,this work demonstrates a simple and effective method to create S vacancies on MoS2,providing theoretical and technical support for the industrial application of MoS2 cata-lysts.

关键词

MoS2纳米片/H2O2刻蚀/S空位/CO2加氢/甲醇/CO

Key words

MoS2 nanosheets/H2O2 etching/S vacancy/CO2 hydrogenation/methanol/CO

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基金项目

江苏省自然科学基金资助项目(BK20231075)

中央高校基本业务经费资助项目(2023QN1012)

中央高校基本业务经费资助项目(2021QN1046)

中国矿业大学安全学科群自主创新资助项目(2022ZZX03)

江苏省碳达峰碳中和科技创新专项资金资助项目(BE2023852)

出版年

2024
洁净煤技术
煤炭科学研究总院 煤炭工业洁净煤工程技术研究中心

洁净煤技术

CSTPCD北大核心
影响因子:0.893
ISSN:1006-6772
参考文献量6
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