单原子Cu锚定的MoN纳米片双活性位点电化学析氢催化剂的构筑及协同作用机理研究

批准号:
22008207
项目类别:
青年科学基金项目
资助金额:
24.0 万元
负责人:
熊洁
依托单位:
学科分类:
反应工程
结题年份:
2023
批准年份:
2020
项目状态:
已结题
项目参与者:
熊洁
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中文摘要
电化学析氢反应本质上是由质子的吸附还原和吸附氢的脱附两步基元反应组成,传统的单一活性位点析氢电催化剂面临着无法同时提升氢吸附和氢脱附动力学的挑战。本课题拟开发一种氨气辅助泡沫Cu实现高温气相迁移,并被富缺陷MoN纳米片限域捕获的策略,构建出兼具氢吸附能强和吸附能弱的金属Cu单原子锚定的MoN纳米片双活性位点析氢催化剂,实现质子在氢吸附能强的MoN位点迅速还原吸附,并在吸附能弱的Cu单原子位点及时脱附,促使质子在MoN和Cu单位点原子尺度界面处发生反应动力学快速的氢吸附和脱附反应,同时通过优化氨气的流速、泡沫铜的氨化逸出温度、停留时间及MoN载体的缺陷程度,调整原子级分散于MoN载体表面的Cu单位点的形态及覆盖度,实现对氢吸附和脱附之间匹配程度进行精准调控,并结合理论模拟和测试表征,揭示双活性位点间的协同作用机理。本研究将为其它多元过渡金属基析氢电催化剂的设计和性能调控提供重要的科学依据。
英文摘要
The electrochemical hydrogen evolution reaction consists essentially of two elementary steps. First, an electron transfers to the catalyst surface is coupled to a proton adsorption on an empty active site of the catalyst to yield an absorbed hydrogen atom, then the adsorbed hydrogen atom would combine with each other through chemical desorption or couple to a second electron and another proton from the solution to generate hydrogen through electrochemical desorption. Therefore, improving simultaneously the kinetics of hydrogen adsorption and hydrogen desorption remains a great challenge for the traditional hydrogen evolution electrocatalyst with only single active site. This project attempts to develop a novel strategy of ammonia-assisted emitting of copper foam and captured by the defect-rich MoN nanosheets at high temperature to construct Cu single atoms anchored MoN nanosheets as a dual-active site hydrogen evolution catalyst, in which the MoN with strong hydrogen adsorption energy facilitates the rapid proton adsorption and Cu single atom site with weak adsorption energy enables the immediate release of generated hydrogen, enhancing synchronously the catalytic kinetics of hydrogen adsorption and desorption elementary steps. Meanwhile, adjustment of the ammonia flow rate, the ammoniation temperature of ammonia-guided emitting of the copper foam, the treatment residence time and the degree of defects of the MoN skeleton will be conducted to evaluate their influences on the loading content and dispersing morphology at the atomic level of Cu single atoms confined on the surface of MoN scaffold, and also to achieve precise regulation of the matching degree between hydrogen adsorption and desorption. Moreover, unveiling the synergistic mechanism of dual active sites between the Cu single atoms and MoN nanosheets will be probed with the help of both theoretical simulation and various characterization techniques. This study will provide an important scientific basis for the design and property modulation of other multiple-element transition metal-based high performance hydrogen evolution electrocatalysts.
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DOI:10.1016/j.jcis.2022.12.085
发表时间:2022-12
期刊:Journal of colloid and interface science
影响因子:9.9
作者:Zhao Liu;Huawei He;Yuxuan Liu;Yi Zhang;Jiawei Shi;J. Xiong;Shunfa Zhou;Jing Li;L. Fan
通讯作者:Zhao Liu;Huawei He;Yuxuan Liu;Yi Zhang;Jiawei Shi;J. Xiong;Shunfa Zhou;Jing Li;L. Fan
DOI:--
发表时间:2022
期刊:山东化工
影响因子:--
作者:熊洁;刘薇;郭晓萧
通讯作者:郭晓萧
DOI:10.1016/j.egyr.2021.04.017
发表时间:2021-04
期刊:Energy Reports
影响因子:5.2
作者:J. Xiong;Chunyan Yan;Wei Liu;Xiaoxiao Guo;Jie Ma;W. Yi;Minfang Han
通讯作者:J. Xiong;Chunyan Yan;Wei Liu;Xiaoxiao Guo;Jie Ma;W. Yi;Minfang Han
DOI:10.1002/ajoc.202300129
发表时间:2023-05-12
期刊:ASIAN JOURNAL OF ORGANIC CHEMISTRY
影响因子:2.7
作者:Shi,Yijun;Sun,Xinyue;Xiong,Jie
通讯作者:Xiong,Jie
国内基金
海外基金
