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
收藏
页数:13
相关论文
共 41 条
  • [1] Cooperative electrocatalytic alcohol oxidation with electron-proton-transfer mediators
    Badalyan, Artavazd
    Stahl, Shannon S.
    [J]. NATURE, 2016, 535 (7612) : 406 - 410
  • [2] FXR inhibition may protect from SARS-CoV-2 infection by reducing ACE2
    Brevini, Teresa
    Maes, Mailis
    Webb, Gwilym J.
    John, Binu, V
    Fuchs, Claudia D.
    Buescher, Gustav
    Wang, Lu
    Griffiths, Chelsea
    Brown, Marnie L.
    Scott, William E., III
    Pereyra-Gerber, Pehuen
    Gelson, William T. H.
    Brown, Stephanie
    Dillon, Scott
    Muraro, Daniele
    Sharp, Jo
    Neary, Megan
    Box, Helen
    Tatham, Lee
    Stewart, James
    Curley, Paul
    Pertinez, Henry
    Forrest, Sally
    Mlcochova, Petra
    Varankar, Sagar S.
    Darvish-Damavandi, Mahnaz
    Mulcahy, Victoria L.
    Kuc, Rhoda E.
    Williams, Thomas L.
    Heslop, James A.
    Rossetti, Davide
    Tysoe, Olivia C.
    Galanakis, Vasileios
    Vila-Gonzalez, Marta
    Crozier, Thomas W. M.
    Bargehr, Johannes
    Sinha, Sanjay
    Upponi, Sara S.
    Fear, Corrina
    Swift, Lisa
    Saeb-Parsy, Kourosh
    Davies, Susan E.
    Wester, Axel
    Hagstrom, Hannes
    Melum, Espen
    Clements, Darran
    Humphreys, Peter
    Herriott, Jo
    Kijak, Edyta
    Cox, Helen
    [J]. NATURE, 2023, 615 (7950) : 134 - +
  • [3] Estrogen and bone health in men and women
    Cauley, Jane A.
    [J]. STEROIDS, 2015, 99 : 11 - 15
  • [4] Facile synthesis of Ni5P4 nanosheets/nanoparticles for highly active and durable hydrogen evolution
    Chen, Anyin
    Fu, Liang
    Xiang, Wenjun
    Wei, Wei
    Liu, Dan
    Liu, Changlu
    [J]. INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2021, 46 (21) : 11701 - 11710
  • [5] The importance of nickel oxyhydroxide deprotonation on its activity towards electrochemical water oxidation
    Diaz-Morales, Oscar
    Ferrus-Suspedra, David
    Koper, Marc T. M.
    [J]. CHEMICAL SCIENCE, 2016, 7 (04) : 2639 - 2645
  • [6] Dual Tuning of Ni-Co-A (A = P, Se, O) Nanosheets by Anion Substitution and Holey Engineering for Efficient Hydrogen Evolution
    Fang, Zhiwei
    Peng, Lele
    Qian, Yumin
    Zhang, Xiao
    Xie, Yujun
    Cha, Judy J.
    Yu, Guihua
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2018, 140 (15) : 5241 - 5247
  • [7] CoPSe: A New Ternary Anode Material for Stable and High-Rate Sodium/Potassium-Ion Batteries
    Feng, Yutong
    Xu, Mengzhu
    He, Ting
    Chen, Bingjie
    Gu, Feng
    Zu, Lianhai
    Meng, Ruijin
    Yang, Jinhu
    [J]. ADVANCED MATERIALS, 2021, 33 (16)
  • [8] Applications of steroid drugs entrapped in cyclodextrins
    Fenyvesi, Eva
    Puskas, Istvan
    Szente, Lajos
    [J]. ENVIRONMENTAL CHEMISTRY LETTERS, 2019, 17 (01) : 375 - 391
  • [9] Deriving the Turnover Frequency of Aminoxyl-Catalyzed Alcohol Oxidation by Chronoamperometry: An Introduction to Organic Electrocatalysis
    Goes, Shannon L.
    Mayer, Mikayla N.
    Nutting, Jordan E.
    Hoober-Burkhardt, Lena E.
    Stahl, Shannon S.
    Rafiee, Mohammad
    [J]. JOURNAL OF CHEMICAL EDUCATION, 2021, 98 (02) : 600 - 606
  • [10] A Century of Cholesterol and Coronaries: From Plaques to Genes to Statins
    Goldstein, Joseph L.
    Brown, Michael S.
    [J]. CELL, 2015, 161 (01) : 161 - 172