journal article·2022-06-01

High-Voltage Redox Mediator of an Organic Electrolyte for Supercapacitors by Lewis Base Electrocatalysis

Zhe-Fan Wang, Zonglin Yi, Song-Chen Yu, Ya-Feng Fan, Jingxue Li, Lijing Xie, Shou-Chun Zhang, Fangyuan Su, Cheng-Meng Chen

ACS Applied Materials & Interfaces· Volume 14· Issue 21
Publisher page

Abstract

Redox electrolytes for supercapacitors (SCs) have recently sparked widespread interest. Due to the redox reactions within electrolytes, they can achieve high capacitance and long cycle stability. However, the energy density of SCs with redox electrolytes is limited by the narrow applied electrochemical window due to the irreversible side reaction of redox mediators at high potential. To overcome this issue, a redox mediator with a high redox potential, tetrachloridehydroquinone (TCHQ), is added to organic electrolytes to obtain a broad electrochemical window. TCHQ is designed to undergo a dehydrogenation reaction catalyzed by N-doped activated carbon to provide capacitance. The pyrrole N atoms have the highest electrocatalytic activity based on the theoretical calculation of reaction overpotential with predicted reaction pathways due to their Lewis basicity. Benefitting from that, TCHQ shows promising reversibility with a larger electrochemical window (up to 2.7 V). As a result, a higher energy density is obtained when compared to commercial SCs. This study proposes a strategy for designing redox mediators and interfaces of SCs with high energy density and a calculation method of dehydrogenation reaction electrocatalysis.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Supercapacitor Materials and Fabrication · Advanced battery technologies research · Electrocatalysts for Energy Conversion

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

CAS Key Laboratory of Carbon Materials, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, Shanxi, China

University of Chinese Academy of Sciences, Beijing 100049, China

Beijing National Laboratory for Molecular Sciences (BNLMS), CAS Key Laboratory of Molecular Recognition and Function, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China

Center of Biomass Engineering/College of Agronomy and Biotechnology, China Agricultural University, Beijing 100193, China

Funding

Ministry of Science and Technology of the People's Republic of China · Yulin University · Youth Innovation Promotion Association of the Chinese Academy of Sciences · Research and Development Project of Key Core and Common Technology of Shanxi Province · Natural Science Basic Research Program of Shanxi · Dalian National Laboratory for Clean Energy · National Science Foundation for Excellent Young Scholars of China

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