Understanding the Mechanism of High Capacitance in Nickel Hexaaminobenzene-Based Conductive Metal-Organic Frameworks in Aqueous Electrolytes

Lukatskaya, Maria R.; Yang, Xiao-Qing; Feng, Dawei; Bak, Seong-Min; To, John W. F.; Cui, Yi C.; Feldblyum, Jeremy I.; Bao, Zhenan

doi:10.1021/acsnano.0c07292

Title: Understanding the Mechanism of High Capacitance in Nickel Hexaaminobenzene-Based Conductive Metal-Organic Frameworks in Aqueous Electrolytes

Journal Article · Mon Nov 09 00:00:00 EST 2020 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.0c07292· OSTI ID:1716832

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Stanford Univ., CA (United States); Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Stanford Univ., CA (United States); Univ. of Wisconsin, Madison, WI (United States)
Stanford Univ., CA (United States)
State Univ. of New York (SUNY), Albany, NY (United States)

Recently, intrinsically conductive metal-organic frameworks (MOFs) have demonstrated promising performance in fast-charging energy storage applications and may outperform some current electrode materials (e.g., porous carbons) for supercapacitors in terms of both gravimetric and volumetric capacitance. In this report, we examine the mechanism of high capacitance in a nickel hexaaminobenzene-based MOF (NiHAB). Using a combination of in situ Raman and X-Ray absorption spectroscopies, as well as detailed electrochemical studies in a series of aqueous electrolytes, we demonstrate in this work that the charge storage mechanism is in fact a pH-dependent surface pseudocapacitance, and, unlike typical inorganic systems, where transition metals change oxidation state during charge/discharge cycles, NiHAB redox activity is ligand-centered.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Science Foundation (NSF); American Chemical Society Petroleum Research Fund; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704; 32023; AC02-76SF00515; ECCS-1542152; 59835-DNI10

OSTI ID:: 1716832

Alternate ID(s):: OSTI ID: 1779445

Report Number(s):: BNL-220607-2020-JAAM

Journal Information:: ACS Nano, Vol. 14, Issue 11; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
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metal-organic frameworks
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Title: Understanding the Mechanism of High Capacitance in Nickel Hexaaminobenzene-Based Conductive Metal-Organic Frameworks in Aqueous Electrolytes

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