Operando generated copper -based catalyst enabling efficient electrosynthesis of 2,5-bis(hydroxymethyl)furan

被引:10
|
作者
Zhang, Zhaolu [1 ,2 ]
Huang, Kai [3 ]
Qiu, Xinyue [1 ]
Ge, Wangxin [1 ]
Yang, Xiaoling [1 ]
Zhu, Yihua [1 ]
Lian, Cheng [3 ]
Liu, Honglai [3 ]
Jiang, Hongliang [2 ]
Li, Zhong [1 ,2 ]
机构
[1] East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Shanghai 200237, Peoples R China
[2] East China Univ Sci & Technol, Sch Chem Engn, Key Lab Ultrafine Mat, Minist Educ, Shanghai 200237, Peoples R China
[3] East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China
来源
FUNDAMENTAL RESEARCH | 2023年 / 3卷 / 05期
基金
中国国家自然科学基金;
关键词
Electrocatalytic upgrading; Copper-based catalyst; Hydrogenation; Water splitting; Interface structure; TOTAL-ENERGY CALCULATIONS; ELECTROCATALYTIC HYDROGENATION; BIOMASS; CONVERSION; REDUCTION; SURFACE; TRITIATION; OXIDATION; WATER;
D O I
10.1016/j.fmre.2022.01.016
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Electrocatalytic upgrading of biomass-derived platform molecules has emerged as a sustainable and environ-mentally benign route to produce high-value chemicals. The main challenge lies in developing efficient cat-alysts for the selective activation of designated chemical bonds in the presence of various reducible groups. This work demonstrated a high-efficiency electrochemical conversion of 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)furan (BHMF), an important industrial synthetic reagent. A highly porous Cu-based cata-lyst was developed that achieved nearly 100% BHMF selectivity and long-term stability. Through comprehen-sive operando and ex-situ structural characterizations, an electrochemically generated catalyst with abundant Cu/Cu2O interfaces was identified as a catalytically active phase for HMF conversion. Deuterated BHMF, with the potential to produce deuterated drugs, was also synthesized using D2O as the deuterium source. Density func-tional theory calculations show that the Cu/Cu2O interface structure exhibits relatively low energy barriers for the hydrogenation of HMF to BHMF. This work provides insights into the origin of electrocatalytic hydrogenation activity and highlights the promising potential of the electrocatalytic synthesis of high-value chemicals.
引用
收藏
页码:763 / 769
页数:7
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