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NixCo1–x@NixCo1–xO/NCNT as Trifunctional ORR, OER, and HER Electrocatalysts and its Application in a Zn–Air Battery
ACS Applied Materials & Interfaces ( IF 9.5 ) Pub Date : 2023-06-02 , DOI: 10.1021/acsami.3c01947
Rohan Jena 1 , Sohini Bhattacharyya 1 , Neha Bothra 2 , Varchaswal Kashyap 1 , Swapan K Pati 2 , Tapas Kumar Maji 1
Affiliation  

The efficient electrochemical conversion and storage devices can be boosted by the development of cost-effective and durable electrocatalysts. However, simultaneous in-depth understanding of the reaction mechanism is also required. Herein, we report the preparation, characterization, and electrochemical activities of bimetallic NixCo1–x NPs and core–shell NixCo1–x@NixCo1–xO NPs stabilized on N-doped carbon nanotubes (NCNTs). The electrocatalyst is derived from a bimetallic MOF {[Ni0.5Co0.5(bpe)2(N(CN)2)](N(CN)2)·(5H2O)}n (1) via pyrolysis followed by calcination. Pyrolysis of the bimetallic MOF gives rise to bimetallic nanoparticles stabilized on NCNTs, which, when subsequently calcined, leads to the formation of a core–shell structure with a semiconducting oxide shell (NixCo1–xO) encapsulating the NixCo1–x bimetallic NP core. Detailed evaluation of the electrocatalytic performance of NixCo1–x@NixCo1–xO/NCNT proves its worth as a bifunctional catalyst with 380 mV overpotential for oxygen evolution reaction at 10 mA cm–2 current density and 0.87 V (vs RHE) onset for oxygen reduction reaction in the alkaline medium. Additionally, the prepared electrocatalyst efficiently catalyzes the hydrogen evolution reaction with a nominal overpotential of 74 mV (vs RHE) for reaching 10 mA cm–2 current density in acidic medium. The practical applicability of this catalyst is further upheld in the fabrication of a zinc–air battery having high specific capacity with high round-trip efficiency and adequate cycle life. DFT calculations establish that the structure of NixCo1–x@NixCo1–xO/NCNT is crucial for its electrochemical activity since it has the threefold advantages of cooperative charge transfer from Co to Ni, synergistic relationship between the conductive alloy core and semiconducting oxide shell, and a highly conductive N-doped CNT matrix.

中文翻译:

NixCo1–x@NixCo1–xO/NCNT 作为三功能 ORR、OER 和 HER 电催化剂及其在锌空气电池中的应用

通过开发具有成本效益和耐用的电催化剂,可以促进高效的电化学转换和存储设备。然而,同时也需要对反应机理有深入的了解。在此,我们报告了稳定在 N 掺杂碳纳米管 (NCNT) 上的双金属 Ni x Co 1– x NPs 和核壳 Ni x Co 1– x @Ni x Co 1– x O NPs的制备、表征和电化学活性. 该电催化剂来源于双金属MOF {[Ni 0.5 Co 0.5 (bpe) 2 (N(CN) 2 )](N(CN) 2 )·(5H2 O)} n (1) 通过热解然后煅烧。双金属 MOF 的热解产生稳定在 NCNT 上的双金属纳米粒子,随后煅烧时,导致形成具有半导体氧化物壳(Ni x Co 1– x O)的核壳结构,封装Ni x Co 1 – x 双金属 NP 内核。对 Ni x Co 1– x @Ni x Co 1– x O/NCNT电催化性能的详细评估证明了其作为双功能催化剂的价值,在 10 mA cm –2下析氧反应的过电位为 380 mV碱性介质中氧还原反应的电流密度和 0.87 V(相对于 RHE)开始。此外,所制备的电催化剂可有效催化析氢反应,标称过电位为 74 mV(相对于 RHE),可在酸性介质中达到 10 mA cm –2电流密度。这种催化剂的实际适用性在制造具有高比容量、高往返效率和足够循环寿命的锌空气电池中得到进一步支持。DFT 计算确定了 Ni x Co 1– x @Ni x Co 1– x的结构O/NCNT 对其电化学活性至关重要,因为它具有从 Co 到 Ni 的协同电荷转移、导电合金核和半导体氧化物壳之间的协同关系以及高导电性 N 掺杂 CNT 基质的三重优势。
更新日期:2023-06-02
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