journal article·2024-12-13

Unraveling the Charge Storage Mechanism of β-MnO2 in Aqueous Zinc Electrolytes

LangYuan Wu, ZhiWei Li, YuXuan Xiang, WenDi Dong, HaiYang Wu, YingHong Xu, ZhenXiao Ling, Munseok S. Chae, Daniel Sharon, Netanel Shpigel, XiaoGang Zhang

ACS Energy Letters· Volume 9· Issue 12
Publisher page

Abstract

MnO 2 -based zinc-ion batteries have emerged as a promising candidate for next-generation energy storage systems. Despite extensive research on MnO 2 electrodes, the charging mechanism in mildly acidic electrolytes remains debated. Most studies have focused on α-MnO 2, and this study aims to shed light on the identity of the charge carrier in β-MnO 2 and the role of the Mn 2+ cations. By employing in situ EQCM-D measurements, along with ssNMR, XRD, TEM, and in situ pH monitoring, we demonstrated that the charging mechanism is primarily governed by proton de/intercalation. Compared to α-MnO 2, with its larger 2 × 2 tunnels that accommodate hydronium ions, the β-phase has smaller 1 × 1 tunnels, permitting only the insertion of bare protons. During cycling, we observed the formation of new phases on β-MnO 2 originating from the repetitive electrodeposition/dissolution of Mn 2+ . In addition, these phases can reversibly host hydronium ions, resulting in a mixed charging mechanism that involves the insertion of both H 3 O + and H + .
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Research context

OpenAlex topics: Advanced battery technologies research · Advanced Battery Materials and Technologies · Supercapacitor Materials and Fabrication

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

Affiliations

Jiangsu Key Laboratory of Materials and Technologies for Energy Storage, College of Materials Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, P. R. China

Department of Chemical Sciences, Ariel University, Ariel 40700, Israel

Research Center for Industries of the Future, Westlake University, Hangzhou, Zhejiang 310030, P. R. China

School of Engineering, Westlake University, Hangzhou, Zhejiang 310030, P. R. China

Department of Nanotechnology Engineering, Pukyong National University, Busan 48513, Republic of Korea

Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem 9190401, Israel

Key Laboratory for Intelligent Nano Materials and Devices of the Ministry of Education, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, P. R. China

Funding

Priority Academic Program Development of Jiangsu Higher Education Institutions · Westlake Education Foundation · Leading Edge Technology of Jiangsu Province

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