Intermetallic RNi2Si2 (R = Ca, La, and Y) Catalysts with Electron-Rich Ni Sites for Continuous Flow Selective Hydrogenation of Maleic Anhydride

被引:0
作者
Zhong, Ying [1 ]
Chen, Xiao [1 ]
Liu, Shiyao [1 ]
Liu, Huibin [1 ]
Hu, Deng [2 ]
Lafaye, Gwendoline [3 ]
Liang, Changhai [1 ]
机构
[1] Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, Lab Adv Mat & Catalyt Engn, Dalian 116024, Peoples R China
[2] Chinese Acad Sci, Shanghai Adv Res Inst, Photon Sci Res Ctr Carbon Dioxide, Shanghai 201210, Peoples R China
[3] Univ Poitiers, Inst Chim Milieux, CNRS, Mat Poitiers IC2MP, F-86073 Poitiers, France
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
intermetallic compound; electron-rich Ni active sites; selective hydrogenation; maleic anhydride; gamma-butyrolactone; AQUEOUS-PHASE HYDROGENATION; TOTAL-ENERGY CALCULATIONS; ACID; SPECTROSCOPY; SILICA; ZN; ZR; CU;
D O I
10.1021/acsami.4c15049
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
The industrial advancement of downstream products resulting from the directed hydrogenation of maleic anhydride is hindered by the limitations related to the activity and stability of catalysts. The development of nonprecious metal intermetallic compounds, in which active sites are adjustable in the local structures and electronic properties embedded within a distinct framework, holds immense potential in enhancing catalytic efficacy and stability. Herein, we report that nickel-based silicides catalysts, RNi2Si2 (R = Ca, La, and Y), afford high efficiency in the selective hydrogenation of maleic anhydride. Among the RNi(2)Si(2 )with the same tetragonal structure, CaNi2Si2 with complete isolation and highest electron density of Ni sites presents the low apparent activation energy (98.4 kJ/mol). Preferential adsorption of intermediate succinic anhydride via C=O bonds is achieved by the high oxygen affinity of CaNi2Si2, resulting in chemoselectivity to gamma-butyrolactone (>80%). Additionally, the silicide with good resistance to sintering and acid corrosion presents remarkable stability for at least 130 h. The design of the silicide structure will offer fresh perspectives on the development of effective and enduring selective hydrogenation catalysts.
引用
收藏
页码:6175 / 6187
页数:13
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