Ultra-small β-Ni(OH)2 quantum dot catalyst with abundant edges for an efficient urea oxidation reaction†

IF 6.4 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Inorganic Chemistry Frontiers Pub Date : 2025-04-17 DOI:10.1039/D5QI00372E
Qishuang Zhu, Xianshu Qiao, Chuanjin Tian, Pengzhang Li, Yumin Liu, Wenyan Zhao, Liang Ma and Chang-An Wang
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Abstract

The development of efficient nonprecious-metal catalysts for the urea oxidation reaction (UOR) to improve the efficiency of electrocatalytic water splitting for hydrogen production remains a challenge. Herein, we synthesized ultra-small β-Ni(OH)2 quantum dot (US-β-Ni(OH)2 QD) catalysts with abundant edges via a coupled co-precipitation and anion-exchange approach. The obtained US-β-Ni(OH)2 QD catalyst exhibits high activity toward the UOR and required a potential of only 1.48 V (vs. RHE) to reach 151 mA cm−2. Notably, the US-β-Ni(OH)2 QD catalyst exhibits 4.1 and 96 times higher current density than do β-Ni(OH)2 nanosheets (38.34 mA cm−2) and a Pt mesh electrode (1.57 mA cm−2), respectively, at a potential of 1.48 V (vs. RHE). The UOR catalytic reaction mechanism reveals that the US-β-Ni(OH)2 QD catalyst features a high density of edge sites, where the oxygen vacancy concentration far exceeds that of the basal plane. This unique oxygen-vacancy-rich edge structure endows the US-β-Ni(OH)2 QDs with a low energy barrier (0.96 eV) for the self-oxidation of Ni(OH)2 to NiOOH, thereby facilitating the rate-determining step of the entire urea degradation process. This work provides a new approach for synthesizing ultra-small hydroxide quantum dot catalysts with efficient UOR activity at low cost.

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具有丰富边缘的超小β-Ni(OH)2量子点催化剂用于高效尿素氧化反应
开发用于尿素氧化反应(UOR)的高效非贵金属催化剂以提高电催化水分离制氢的效率仍然是一项挑战。在此,我们采用共沉淀和阴离子交换的耦合方法合成了一种具有丰富边缘的超小型β-Ni(OH)2量子点催化剂(US-β-Ni(OH)2 QDs)。获得的 US-β-Ni(OH)2 QDs 催化剂对 UOR 具有很高的活性,所需的电位仅为 1.48 V(相对于 RHE),即可达到 151 mA-cm-2。值得注意的是,US-β-Ni(OH)2 QDs 催化剂在 1.48 V 电位(相对于 RHE)下的电流密度分别是 β-Ni(OH)2 纳米片(38.34 mA cm-2)和铂网电极(1.57 mA cm-2)的 4.1 倍和 96 倍。催化反应机理表明,与β-Ni(OH)2纳米片相比,超小尺寸(约3 nm)的US-β-Ni(OH)2 QDs催化剂具有更丰富的边缘,这为催化反应提供了丰富的活性位点。此外,研究还发现 US-β-Ni(OH)2 QDs 边缘的 Ni-OH 键比β-Ni(OH)2 纳米片的边缘和基面更活跃,能促进 Ni2+ 向 Ni3+ 的转化和尿素分子的吸附,降低 UOR 反应的能垒,从而提高 UOR 性能。这项工作为合成具有高效 UOR 活性且成本低廉的超小氢氧化物量子点催化剂提供了一种新方法。
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来源期刊
Inorganic Chemistry Frontiers
Inorganic Chemistry Frontiers CHEMISTRY, INORGANIC & NUCLEAR-
CiteScore
10.40
自引率
7.10%
发文量
587
审稿时长
1.2 months
期刊介绍: The international, high quality journal for interdisciplinary research between inorganic chemistry and related subjects
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