PMID- 36642694 OWN - NLM STAT- PubMed-not-MEDLINE DCOM- 20230228 LR - 20230228 IS - 1521-3773 (Electronic) IS - 1433-7851 (Linking) VI - 62 IP - 11 DP - 2023 Mar 6 TI - Boosting Hydrogen Production via Selective Two-electron Mild Electrochemical Oxidation of Tetrahydroisoquinolines Completely to Dihydroisoquinolines. PG - e202216347 LID - 10.1002/anie.202216347 [doi] AB - Different from the previous study that biomass derivatives replace water oxidation for enhancing hydrogen production, we found that mild oxidation was more conductive to cathodic hydrogen production. In this study, maximum Faradaic efficiency (>99 %) and lower energy consumption for hydrogen production was achieved by precisely controlling the two-electron mild electrochemical oxidation of tetrahydroisoquinolines (THIQs) to dihydroisoquinolines (DHIQs) in place of the four-electron deep oxidation to isoquinolines (IQs). Moreover, the high value-added DHIQs were prepared from THIQs with high selectivity (>99 %) at the low potential of 1.36 V. Operando electrochemical Raman and density functional theory proved that the high selectivity was attributed to the regulable active species of NiOOH induced by the interaction of Co and Fe for preferentially breaking C-H bond rather than N-H of THIQs. This novel method provides important insight into efficient biomass-assisted hydrogen production. CI - (c) 2023 Wiley-VCH GmbH. FAU - Zhou, Zhaoyu AU - Zhou Z AD - School of Chemical Science and Engineering, Shanghai Key Lab of Chemical Assessment and Sustainability, Tongji University, 1239 Siping Road, Shanghai, 200092, P. R. China. FAU - Pan, Xun AU - Pan X AD - School of Chemical Science and Engineering, Shanghai Key Lab of Chemical Assessment and Sustainability, Tongji University, 1239 Siping Road, Shanghai, 200092, P. R. China. FAU - Sun, Lingzhi AU - Sun L AD - School of Chemical Science and Engineering, Shanghai Key Lab of Chemical Assessment and Sustainability, Tongji University, 1239 Siping Road, Shanghai, 200092, P. R. China. FAU - Xie, Yanan AU - Xie Y AD - School of Chemical Science and Engineering, Shanghai Key Lab of Chemical Assessment and Sustainability, Tongji University, 1239 Siping Road, Shanghai, 200092, P. R. China. FAU - Zheng, Jingui AU - Zheng J AD - School of Chemical Science and Engineering, Shanghai Key Lab of Chemical Assessment and Sustainability, Tongji University, 1239 Siping Road, Shanghai, 200092, P. R. China. FAU - Li, Lina AU - Li L AD - Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Shanghai, 201800, P. R. China. FAU - Zhao, Guohua AU - Zhao G AUID- ORCID: 0000-0002-8693-1193 AD - School of Chemical Science and Engineering, Shanghai Key Lab of Chemical Assessment and Sustainability, Tongji University, 1239 Siping Road, Shanghai, 200092, P. R. China. LA - eng GR - 22076140/National Natural Science Foundation of China/ GR - 21876128/National Natural Science Foundation of China/ GR - 21537003/National Natural Science Foundation of China/ GR - 2022-SSRF-PT-020439/Shanghai Synchrotron Radiation Facility/ GR - 2022-SSRF-PT-020432/Shanghai Synchrotron Radiation Facility/ PT - Journal Article DEP - 20230201 PL - Germany TA - Angew Chem Int Ed Engl JT - Angewandte Chemie (International ed. in English) JID - 0370543 SB - IM OTO - NOTNLM OT - Hydrogen Production OT - Mild Oxidation OT - NiOOH Species OT - Operando Technologies OT - Selective Conversion EDAT- 2023/01/16 06:00 MHDA- 2023/01/16 06:01 CRDT- 2023/01/15 22:12 PHST- 2022/11/06 00:00 [received] PHST- 2023/01/16 06:00 [pubmed] PHST- 2023/01/16 06:01 [medline] PHST- 2023/01/15 22:12 [entrez] AID - 10.1002/anie.202216347 [doi] PST - ppublish SO - Angew Chem Int Ed Engl. 2023 Mar 6;62(11):e202216347. doi: 10.1002/anie.202216347. Epub 2023 Feb 1.