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负载于磷化碳氮化物骨架上的单前驱体衍生的亚1纳米钼钴双金属颗粒用于可持续制氢

Single Precursor-Derived Sub-1 nm MoCo Bimetallic Particles Decorated on Phosphide-Carbon Nitride Framework for Sustainable Hydrogen Generation.

作者信息

Hussain Sadam, Sohail Manzar, Shahzad Nadia, Will Geoffrey, O'Mulane Anthony P, Abdala Ahmed, Alnaser Ibrahim A, Karim Mohammad Rezaul, Wahab Md Abdul

机构信息

Department of Chemistry, School of Natural Sciences, National University of Sciences and Technology (NUST), Islamabad 44000, Pakistan.

U.S.-Pakistan Center for Advanced Studies in Energy (USPCAS-E), National University of Sciences and Technology (NUST), Islamabad 44000, Pakistan.

出版信息

ACS Appl Mater Interfaces. 2025 Jan 22;17(3):4728-4743. doi: 10.1021/acsami.4c12577. Epub 2025 Jan 8.

DOI:10.1021/acsami.4c12577
PMID:39779368
Abstract

The strategic design and fabrication of efficient electrocatalysts are pivotal for advancing the field of electrochemical water splitting (EWS). To enhance EWS performance, integrating non-noble transition metal catalysts through a cooperative double metal incorporation strategy is important and offers a compelling alternative to conventional precious metal-based materials. This study introduces a novel, straightforward, single-step process for fabricating a bimetallic MoCo catalyst integrated within a three-dimensional (3D) nanoporous network of N, P-doped carbon nitride derived from a self-contained precursor. The subsequent carbonization at 550 °C yields a highly effective bimetallic phosphide carbon nitride electrocatalyst, denoted as MoCoPCN, tailored explicitly for EWS. The MoCoPCN electrocatalyst demonstrates exceptional electrocatalytic performance, with a low onset potential of 1.43 V and an overpotential value of 202 mV at a current density of 10 mA/cm for the oxygen evolution reaction (OER) and 49.5 mV for the hydrogen evolution reaction (HER), respectively. Moreover, the catalyst exhibits a high electrochemically active surface area of 2720 cm, a small Tafel slope of 47.5 mV dec for HER and 45.7 mV dec for the OER, and a low charge transfer resistance of 0.09 Ω for the HER and 0.805 Ω for the OER. The optimal catalyst was tested for overall water splitting performance in a 1 M KOH electrolyte, demonstrating excellent efficiency with a low cell voltage of 1.49 V required to achieve a current density of 10 mA/cm. These outstanding characteristics, combined with the synergistic effects arising from the interaction between MoCo and P--CN (PCN), underscore the potential of a bimetallic phosphide carbon nitride material as a highly promising electrocatalyst for efficient water splitting.

摘要

高效电催化剂的战略设计与制备对于推动电化学水分解(EWS)领域的发展至关重要。为了提高EWS性能,通过协同双金属掺入策略整合非贵金属过渡金属催化剂很重要,并且为传统的贵金属基材料提供了一个有吸引力的替代方案。本研究介绍了一种新颖、简单的单步工艺,用于制备一种双金属MoCo催化剂,该催化剂集成在由自含前驱体制备的三维(3D)氮、磷掺杂氮化碳纳米多孔网络中。随后在550℃碳化得到一种高效的双金属磷化物氮化碳电催化剂,记为MoCoPCN,专门为EWS量身定制。MoCoPCN电催化剂表现出优异的电催化性能,在析氧反应(OER)中,起始电位低至1.43 V,在电流密度为10 mA/cm²时过电位值为202 mV,在析氢反应(HER)中过电位值为49.5 mV。此外,该催化剂具有2720 cm²的高电化学活性表面积,HER的塔菲尔斜率小至47.5 mV dec⁻¹,OER的塔菲尔斜率为45.7 mV dec⁻¹,HER的电荷转移电阻低至0.09 Ω,OER的电荷转移电阻为0.805 Ω。在1 M KOH电解液中测试了最佳催化剂的全水分解性能,在电流密度为10 mA/cm²时,仅需1.49 V的低电池电压,显示出优异的效率。这些突出的特性,再加上MoCo与P-CN(PCN)之间相互作用产生的协同效应,凸显了双金属磷化物氮化碳材料作为一种极具前景的高效水分解电催化剂的潜力。

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