文献类型：期刊文献

英文题名：Theoretical study on dry reforming of methane catalyzed by Cu12M (M = Cu, Fe, Co, Ni) core-shell bimetallic clusters

作者：Zhang, Lianyang[1];Meng, Yue[2,5];Yang, Jianming[3];Shen, Hui[3];Yang, Chunfang[3];Xie, Bo[4];Xia, Shengjie[4]

机构：[1]Shaoxing Univ, Coll Text & Fash, Key Lab Clean Dyeing & Finishing Technol Zhejiang, Shaoxing 312000, Zhejiang, Peoples R China;[2]Huzhou Univ, Sch Life Sci, 759 East Erhuan Rd, Huzhou 313000, Peoples R China;[3]Zhejiang Huayuan Pigment Co Ltd, Deqing 310024, Zhejiang, Peoples R China;[4]Zhejiang Univ Technol, Dept Chem, Coll Chem Engn, 18 Chaowang Rd, Hangzhou 310014, Peoples R China;[5]Huzhou Coll, Dept Life & Hlth Sci, Huzhou 313000, Peoples R China

年份：2021

卷号：303

外文期刊名：FUEL

收录：SCI-EXPANDED(收录号：WOS:000688588600010)、、EI(收录号：20212710592768)、Scopus(收录号：2-s2.0-85109016511)、WOS

基金：This work is supported by National Natural Science Foundation of China (92061126, 51871091, 21503188) , Opening Project of Key Lab-oratory of Clean Dyeing and Finishing Technology of Zhejiang Province (QJRZ1901) and Zhejiang Leading Innovation and Entrepreneurship Team Project (2018R01008) .

语种：英文

外文关键词：Dry reforming of methane (DRM); Density functional theory (DFT); Alloy; Core-shell structure; Reaction mechanism

外文摘要：Dry reforming of methane (DRM) reaction can not only effectively solve the greenhouse effect, but also produce H2 and CO, which are important raw materials and intermediates for Fischer-Tropsch synthesis. In this paper, the mechanism of DRM on Cu12M (M = Cu, Fe, Co, Ni) core-shell bimetallic nanoclusters was studied by density functional theory (DFT). The Mulliken charge distribution indicates that the charge in the core-shell structure is transferred to the shell atom (Fe, Co, Ni) through the core atom (Cu). The results of binding energy and bond length indicate that Fe, Co and Ni as core atoms enhance the structural stability of Cu13 nanoclusters. The analysis of partial density of states (PDOS) and d-band center indicates that Cu12Ni is the most potential DRM catalyst due to the highest electronic activity. The mechanism study shows that Cu13, Cu12Co and Cu12Ni all react in the same path, while Cu12Fe takes another route. The rate-determining step is CH3* -> CH2* + H*, and the total energy barrier of DRM on Cu12Ni nanocluster is relatively the lowest, which is the most cluster to catalytic DRM reaction.