Highly efficient electrocatalytic oxidation of sterol by synergistic effect of aminoxyl radicals and Se-Ni5P4

被引:4
作者
He, Jiahui [1 ]
Li, Suiqin [1 ]
Li, Chun [2 ]
Li, Kai [1 ]
Xu, Yinjie [1 ]
Wang, Mengxin [1 ]
Zhao, Shuying [1 ]
Zhang, Jiefeng [2 ]
Zhong, Xing [1 ,3 ]
Li, Xiaonian [1 ]
Zhang, Zhengbin [2 ,4 ]
Wang, Jianguo [1 ,3 ]
机构
[1] Zhejiang Univ Technol, Inst Ind Catalysis, State Key Lab Breeding Base Green Chem Synth Techn, Hangzhou, Peoples R China
[2] Zhejiang Xianju Junye Pharmaceut Co Ltd, Res & Dev Dept, Taizhou, Peoples R China
[3] Zhejiang Univ Technol, Inst Ind Catalysis, State Key Lab Breeding Base Green Chem Synth Techn, Hangzhou 310032, Peoples R China
[4] Zhejiang Xianju Junye Pharmaceut Co Ltd, Res & Dev Dept, Taizhou 317300, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
aminoxyl radicals; electrochemical alcohol oxidation; process intensification; stacked electrolyzer; sterol; ALCOHOL OXIDATION; BIFUNCTIONAL ELECTROCATALYST; NANOPARTICLES;
D O I
10.1002/aic.18153
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
The exploration of efficient and environmentally friendly oxidation method is highly desirable to overcome the critical problems of poor selectivity and heavy metal contamination for the fine chemicals industry. Herein, a self-supported three-dimensional (3D) Se-Ni5P4 nanosheet electrocatalyst was rationally designed and fabricated. Benefiting from the synergistic effect of aminoxyl radical and mesoporous Se-Ni5P4/graphite felt (GF), an excellent performance of =98% selectivity and 33.12 kg (m(-3) h(-1)) space-time yield was obtained for sterol intermediate oxidation with the enhanced mass transfer effect of the continuous flow system. The doping of anionic selenium and phosphorus modulated the electronic structure of Se-Ni5P4, and the oxyhydroxides generated by surface reconstruction accelerated the turnover of 2,2,6,6-tetramethyl-1-piperidine N-oxyl (TEMPO), thereby enhancing the intrinsic electrocatalytic activity. A scale-up experiment was conducted with stacked-flow electrolyzer demonstrated the application potential. This work provided an efficient synergistic electrocatalytic strategy to facilitate rapid electron and mass transfer for electrochemical alcohol oxidation and highlighted the potential for practical electrosynthesis applications.
引用
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页数:13
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