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Electronic Structure Modification of MnO2 Nanosheet Arrays with Enhanced Water Oxidation Activity and Stability by Nitrogen Plasma

ACS APPLIED MATERIALS & INTERFACES(2024)

Hebei Univ Technol

Cited 0|Views6
Abstract
The strategic design of catalysts for the oxygen evolution reaction (OER) is crucial in tackling the substantial energy demands associated with hydrogen production in electrolytic water splitting. Despite extensive research on birnessite (delta-MnO2) manganese oxides to enhance catalytic activity by modulating Mn3+ species, the ongoing challenge is to simultaneously stabilize Mn3+ while improving overall activity. Herein, oxygen (O) vacancies and nitrogen (N) doping have been simultaneously introduced into the MnO2 through a simple nitrogen plasma approach, resulting in efficient OER performance. The optimized N-MnO2 v electrocatalyst exhibits outstanding OER activity in alkaline electrolyte, reducing the overpotential by nearly 160 mV compared to pure pristine MnO2 (from 476 to 312 mV) at 10 mA cm(-2), and a small Tafel slope of 89 mV dec(-1). Moreover, it demonstrates excellent durability over a 122 h stability test. The introduction of O vacancies and incorporation of N not only fine-tune the electronic structure of MnO2, increasing the Mn3+ content to enhance overall activity, but also play a crucial role in stabilizing Mn3+, thereby leading to exceptional stability over time. Subsequently, density functional theory calculations validate the optimized electronic structure of MnO(2 )achieved through the two engineering methods, effectively lowering the intermediate adsorption free energy barrier. Our synergistic approach, utilizing nitrogen plasma treatment, opens a pathway to concurrently enhance the activity and stability of OER electrocatalysts, applicable not only to Mn-based but also to other transition metal oxides.
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birnessite,electronic structure modification,nitrogen plasma,oxygen evolution reaction,activityand stability
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要点】:该论文提出了一种利用氮等离子体技术同时引入氧空位和氮掺杂的MnO2纳米片阵列,显著提高了其在碱性电解质中的水分解氧析出反应(OER)活性和稳定性。

方法】:通过氮等离子体处理方法在MnO2中同时引入氧空位和氮原子掺杂,调节电子结构并增加Mn3+含量。

实验】:使用氮等离子体处理后的N-MnO2 v电催化剂在碱性电解质中展示了卓越的OER性能,达到10 mA cm(-2)的电流密度时,过电位降低了160 mV(从原始MnO2的476 mV降至312 mV),Tafel斜率仅为89 mV dec(-1),并在122小时的稳定性测试中表现出优异的耐久性。通过密度泛函理论计算验证了两种工程方法优化后的MnO2电子结构,有效降低了中间产物吸附的自由能垒。