利用高熵五元合金接枝炭黑对水解介导制氢的综合见解

IF 9.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL
Gokul Raj, Ravi Nandan, Soumen Midya, Kanhai Kumar, Abhishek Kumar Singh and Karuna Kar Nanda
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引用次数: 0

摘要

氢是一种很有前途的燃料,具有足够的能量密度和燃烧时的零碳排放。以硼氢化钠(NaBH4)等富氢材料为原料,快速、方便地制备硼氢化钠具有重要的现实意义。本文报道了一种负载导电碳(HEACB)的新型五重高熵crmnnfeconi合金,作为室温下NaBH4水解制氢的有效非均相催化剂。优化后的HEACB具有良好的性能,翻转频率(TOF)约为188 mL gMn−1 s−1,最小活化能(Ea)约为15 kJ mol−1,而裸HEA的活化能为43 kJ mol−1。Mott-Schottky分析揭示了反应过程中HEACB异质结构在电解质界面处的n型半导体行为,具有最佳的平带电位。电化学分析用于了解水解过程中观察到的催化行为的动力学方面。从线性扫描伏安法和电化学阻抗研究中提取的起始电位、过电位、Tafel斜率和电荷转移电阻表明,HEA合金的稳定性对NaBH4水解的整体催化效率有很大影响。化学和电化学研究显示出明显的相关性。应用密度泛函理论(DFT)来理解反应中间体的相互作用,并对硼氢化物在HEA体系上的水解过程提供见解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Comprehensive insights into hydrolysis-mediated hydrogen production using high-entropy quintuple alloy-grafted carbon black†

Comprehensive insights into hydrolysis-mediated hydrogen production using high-entropy quintuple alloy-grafted carbon black†

Comprehensive insights into hydrolysis-mediated hydrogen production using high-entropy quintuple alloy-grafted carbon black†

Hydrogen is a promising fuel with adequate energy density and zero carbon emissions upon combustion. Its fast and convenient production from hydrogen-rich materials like sodium borohydride (NaBH4) is of high practical importance. Herein, we report a novel quintuple high-entropy alloy of CrMnFeCoNi loaded on conductive carbon (HEACB) as an effective heterogeneous catalyst for the hydrolysis of NaBH4 to produce hydrogen at room temperature. The optimized HEACB shows excellent performance with a turn over freequency (TOF) of about 188 mL gMn−1 s−1 and a minimum activation energy (Ea) of about 15 kJ mol−1, while the Ea of bare HEA is 43 kJ mol−1. Mott–Schottky analysis reveals n-type semiconductor behavior of the HEACB heterostructure at the electrolyte interface during the reaction with an optimal flat band potential. Electrochemical analysis is employed to understand the kinetic aspects of the observed catalytic behavior during hydrolysis. The onset potential, overpotential, Tafel slope, and charge transfer resistance extracted from linear sweep voltammetry and electrochemical impedance studies reveal that the HEA alloy stabilization greatly affects the overall catalytic efficiency towards NaBH4 hydrolysis. Chemical and electrochemical investigations exhibit a pronounced correlation. Density Functional Theory (DFT) is applied to understand the interaction of the reaction intermediates and to provide insights into the hydrolysis process of borohydride on the HEA system.

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来源期刊
Journal of Materials Chemistry A
Journal of Materials Chemistry A CHEMISTRY, PHYSICAL-ENERGY & FUELS
CiteScore
19.50
自引率
5.00%
发文量
1892
审稿时长
1.5 months
期刊介绍: The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.
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