气候变化领域集成服务门户(CCPortal): Building a stable cationic molecule/electrode interface for highly efficient and durable CO2reduction at an industrially relevant current

CCPortal

DOI	10.1039/d0ee02535f
	Building a stable cationic molecule/electrode interface for highly efficient and durable CO2reduction at an industrially relevant current
	Su J.; Zhang J.-J.; Chen J.; Song Y.; Huang L.; Zhu M.; Yakobson B.I.; Tang B.Z.; Ye R.
发表日期	2021
ISSN	17545692
起始页码	483
结束页码	492
卷号	14 期号:1
英文摘要	Aggregation and leaching are two major obstacles to the synthesis of efficient and durable heterogeneous molecular catalysts. These problems are even more severe for charged molecules, not only resulting in unsatisfactory performance, but also leading to misleading evaluation of charged functionalities. In this work, methylation of cobalt(ii) tetraamino phthalocyanine (CoTAPc) transforms its electron-donating amino groups into electron-withdrawing quaternary ammonium cations, which favor the formation of COOH intermediate and the desorption of CO; this is conducive to a 130% increase of the current density for the CO2 reduction reaction (CO2RR). However, the catalysts leach severely; consequently, the current density decays rapidly. To resolve this dilemma, we developed an in situ functionalization strategy by first covalently grafting CoTAPc onto carbon nanotubes via a diazo-reaction, followed by a complete methylation reaction. This is conducive to a 700% increase in CO partial current density compared to that of a physically mixed sample at-0.72 V vs. RHE with highly stable currents. In a flow cell, this covalently immobilized structure delivers an industrially relevant current density of 239 mA cm-2, CO selectivity of 95.6% at 590 mV overpotential and very low molecular loading of 0.069 mg cm-2. This work provides mechanistic insight and a design strategy for charged molecular catalysts for high-performance and stable heterogeneous electrolysis. © The Royal Society of Chemistry.
英文关键词	Alkylation; Catalysts; Current density; Grafting (chemical); Leaching; Methylation; Molecules; Cationic molecules; Current density decay; Electronwithdrawing; Functionalizations; Methylation reaction; Molecular catalysts; Molecular loadings; Quaternary ammonium; Cobalt compounds; catalyst; cation; electrode; energy efficiency; in situ measurement; methylation; molecular analysis; performance assessment; reduction
语种	英语
来源期刊	Energy & Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/190809
作者单位	Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Hong Kong, 999077, Hong Kong; Department of Materials Science and Nano Engineering, Rice University, 6100 Main Street, Houston, TX 77005, United States; State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China; Department of Chemistry, Hong Kong Br. of Chinese Natl. Eng. Res. Ctr. for Tissue Restoration and Reconstr. and Inst. for Adv. Stud., SCUT-HKUST Joint Research Institute, Hong Kong University of Science and Technology Clear Water Bay, Kowloon, 999077, Hong Kong; HKUST-Shenzhen Research Institute, No. 9 Yuexing 1st Rd South Area Hi-tech Park Nanshan, Shenzhen, 518057, China; Center for Aggregation-Induced Emission, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology Tianhe Qu, Guangzhou, 510640, China; City University of Hong Kong Shenzhen Research Institute, Shenzhen Guangdong, 518057, China
推荐引用方式 GB/T 7714	Su J.,Zhang J.-J.,Chen J.,et al. Building a stable cationic molecule/electrode interface for highly efficient and durable CO2reduction at an industrially relevant current[J],2021,14(1).
APA	Su J..,Zhang J.-J..,Chen J..,Song Y..,Huang L..,...&Ye R..(2021).Building a stable cationic molecule/electrode interface for highly efficient and durable CO2reduction at an industrially relevant current.Energy & Environmental Science,14(1).
MLA	Su J.,et al."Building a stable cationic molecule/electrode interface for highly efficient and durable CO2reduction at an industrially relevant current".Energy & Environmental Science 14.1(2021).