Doping-modulated strain control of bifunctional electrocatalysis for rechargeable zinc–air batteries,Energy & Environmental Science

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Doping-modulated strain control of bifunctional electrocatalysis for rechargeable zinc–air batteries
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2021-07-27 , DOI: 10.1039/d1ee01271a
Zhao Li _{1,

2} , Qi Wang ₃ , Xiaowan Bai ₄ , Maoyu Wang ₅ , Zhenzhong Yang ₆ , Yingge Du ₆ , George E. Sterbinsky ₇ , Duojie Wu ₃ , Zhenzhen Yang ₈ , Huajun Tian ₁ , Fuping Pan ₁ , Meng Gu ₃ , Yuanyue Liu ₄ , Zhenxing Feng ₅ , Yang Yang _{1,

2,

9,

10}

Affiliation

NanoScience Technology Center, University of Central Florida, Orlando, FL 32826, USA
Department of Materials Science and Engineering, University of Central Florida, Orlando, FL 32826, USA
Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China
Texas Materials Institute and Department of Mechanical Engineering, The University of Texas at Austin, Austin, Texas 78712, USA
School of Chemical, Biological, and Environmental Engineering, Oregon State University, Corvallis, OR 97331, USA
Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, USA
X-ray Science Division, Advanced Photon Source, Argonne National Laboratory, 9700 S Cass Avenue, Argonne, IL, 60439, USA
Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 S Cass Avenue, Lemont, IL, 60439, USA
Renewable Energy and Chemical Transformation Cluster, University of Central Florida, Orlando, FL 32826, USA
Department of Chemistry, University of Central Florida, Orlando, FL 32826, USA

Changes in the local atomic arrangement in a crystal caused by lattice-mismatch-induced strain can efficiently regulate the performance of electrocatalysts for zinc–air batteries (ZABs) in many manners, mainly due to modulated electronic structure configurations that affect the adsorption energies for oxygen-intermediates formed during oxygen reduction and evolution reactions (ORR and OER). However, the application of strain engineering in electrocatalysis has been limited by the strain relaxation caused by structural instability such as dissolution and destruction, leading to insufficient durability towards the ORR/OER. Herein, we propose a doping strategy to modulate the phase transition and formation of self-supported cobalt fluoride–sulfide (CoFS) nanoporous films using a low amount of copper (Cu) as a dopant. This well-defined Cu–CoFS heterostructure overcomes the obstacle of structural instability. Our study of the proposed Cu–CoFS also helps establish the structure–property relationship of strained electrocatalysts by unraveling the role of local strain in regulating the electronic structure of the catalyst. As a proof-of-concept, the Cu–CoFS electrocatalyst with doping-modulated strain exhibited superior onset potentials of 0.91 V and 1.49 V for the ORR and OER, respectively, surpassing commercial Pt/C@RuO₂ and benchmarking non-platinum group metal (non-PGM) catalysts. ZABs with the Cu–CoFS catalyst delivered excellent charge/discharge cycling performance with an extremely low voltage gap of 0.5 V at a current density of 10 mA cm⁻² and successively 0.93 V at a high current density of 100 mA cm⁻² and afforded an outstanding peak power density of 255 mW cm⁻².

中文翻译：

可充电锌空气电池双功能电催化的掺杂调制应变控制

由晶格失配引起的应变引起的晶体局部原子排列的变化可以通过多种方式有效地调节锌空气电池（ZAB）电催化剂的性能，这主要是由于影响氧吸附能的调制电子结构配置- 在氧还原和析出反应（ORR 和 OER）期间形成的中间体。然而，应变工程在电催化中的应用受到结构不稳定性（如溶解和破坏）引起的应变松弛的限制，导致对 ORR/OER 的耐久性不足。在此，我们提出了一种掺杂策略，以使用少量铜 (Cu) 作为掺杂剂来调节相变和自支撑氟化钴 (CoFS) 纳米多孔薄膜的形成。这种明确定义的 Cu-CoFS 异质结构克服了结构不稳定性的障碍。我们对所提出的 Cu-CoFS 的研究还有助于通过揭示局部应变在调节催化剂电子结构中的作用来建立应变电催化剂的结构 - 性质关系。作为概念验证，具有掺杂调制应变的 Cu-CoFS 电催化剂的 ORR 和 OER 的起始电位分别为 0.91 V 和 1.49 V，超过了商业 Pt/C@RuO₂和基准非铂族金属（非 PGM）催化剂。具有 Cu-CoFS 催化剂的 ZAB 提供了极低的充放电循环性能，在 10 mA cm^-2的电流密度下具有 0.5 V 的极低电压间隙，并在 100 mA cm^-2的高电流密度下连续达到 0.93 V，并提供255 mW cm^-2的出色峰值功率密度。

更新日期：2021-08-11

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