Work Function-Induced Electronic Modulation in NiCo Alloy for Electrochemical Nitrate Reduction

IF 4.7 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR
Yan Shen, Yingnan Dou, Liping Sun*, Lihua Huo and Hui Zhao*, 
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Abstract

The rational design of electrocatalysts is of great significance in the production of ammonia (NH3) through a nitrate reduction reaction (NO3RR). This article proposes a design approach to regulate electron redistribution and intermediate adsorption energy by adjusting the work function of alloy compounds. As an example, the NiCo alloy is successfully electrodeposited on carbon cloth (CC) using deep eutectic solvent (DES) as medium. The results show that the ammonia production rate of the NiCo alloy is as high as 1.55 mmol h–1 cm–2 at −0.38 V vs RHE, with the Faraday efficiency to be 84.94%, and the selectivity 94%. Experimental characterizations combined with density functional theory calculations confirm that alloying is beneficial for reducing the work function of Ni. This in turn adjusts the d-band center of the alloy to approach the Fermi level, changes the rate-determining step during the reduction reaction process, and consequently improves the performance. Eventually, an investigation is conducted on the Zn–NO3 battery fabricated with Ni1Co2/CC. This further exhibits the potential of Ni1Co2/CC within the energy conversion equipment. This study brings fresh design concepts and opportunities to the development of novel electrocatalysts for NO3RR.

Abstract Image

NiCo合金中功函数诱导的电子调制电化学还原硝酸盐
电催化剂的合理设计对硝酸还原反应(NO3-RR)生产氨(NH3)具有重要意义。本文提出了一种通过调节合金化合物的功函数来调节电子重分配和中间吸附能的设计方法。以深共晶溶剂(DES)为介质,成功地在碳布(CC)上电沉积了NiCo合金。结果表明,在−0.38 V vs RHE条件下,NiCo合金的产氨率高达1.55 mmol h-1 cm-2,法拉第效率为84.94%,选择性为94%。实验表征结合密度泛函理论计算证实合金化有利于降低Ni的功函数。这反过来又调整了合金的d带中心,使其接近费米能级,改变了还原反应过程中的速率决定步骤,从而提高了性能。最后,对用Ni1Co2/CC制备Zn-NO3 -电池进行了研究。这进一步展示了Ni1Co2/CC在能量转换设备中的潜力。该研究为新型NO3-RR电催化剂的开发带来了新的设计理念和机遇。
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来源期刊
Inorganic Chemistry
Inorganic Chemistry 化学-无机化学与核化学
CiteScore
7.60
自引率
13.00%
发文量
1960
审稿时长
1.9 months
期刊介绍: Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.
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