Optimizing intermediate adsorption and active hydrogen supply on multi-sites Ru,B co-doped Co3O4 for enhanced nitrate electroreduction to ammonia

IF 13.3 1区 工程技术 Q1 ENGINEERING, CHEMICAL
Xiangyu Wang, Libo Chen, Qianling Wei, Zi Wen, Guopeng Ding, Zixuan Feng, Zhili Wang, Qing Jiang
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引用次数: 0

Abstract

Electrocatalytic nitrate reduction reaction (NO3RR) is a highly attractive route for both nitrate-containing wastewater treatment and sustainable ammonia (NH3) synthesis. However, the efficiency of NO3RR is still too low to meet the requirements for practical applications. Here we report a facile dual doping strategy to construct a multi-sites Ru,B co-doped Co3O4/CNT catalyst, which exhibits an attractive NH3 yield rate of 178.1 mg h−1 mgcat−1 and a high NH3 Faradic efficiency of 97.1 % at −0.1 V vs. RHE, far superior to the Co3O4/CNT (20.1 mg h−1 mgcat−1 and 52.6 %) and most of the reported catalysts under similar conditions. Experiments and density functional theory calculations reveal that the co-doping of Ru and B into Co3O4 can generate multiple active sites, in which the Ru-Co bridge site facilitates the adsorption and activation NO3, the Co atom near B atom boosts the *NO protonation to form *NOH, and meanwhile Ru-B dopants promote H2O dissociation to supply abundant *H for intermediates hydrogenation. The cooperation of different active sites promotes the NO3RR. This work offers an opportunity to design more efficient NO3RR electrocatalysts with potential for practical application.
优化多位点Ru,B共掺杂Co3O4的中间吸附和活性氢供应以增强硝酸盐电还原制氨
电催化硝酸还原反应(NO3 - RR)是处理含硝酸盐废水和可持续合成氨(NH3)的一种极具吸引力的途径。然而,NO3−RR的效率仍然太低,无法满足实际应用的要求。这里我们报告一个灵巧的双掺杂策略构建一个多站点俄文,B co-doped Co3O4 CNT /催化剂,展示一个有吸引力的NH3收益率的178.1 毫克 h−1 mgcat−1和NH3感应电的效率高97.1 % 0.1− V和流值,远优于Co3O4 CNT / (20.1 mg  h−1 mgcat−1和52.6 %)和大部分的报道在类似条件下催化剂。实验和密度泛函理论计算表明,Ru和B共掺杂到Co3O4中可以产生多个活性位点,其中Ru-Co桥位有利于吸附和活化NO3−,靠近B原子的Co原子促进*NO质子化形成*NOH,同时Ru-B掺杂剂促进H2O解离,为中间体加氢提供丰富的*H。不同活性位点的协同作用促进了NO3−RR的发生。这项工作为设计具有实际应用潜力的更高效的NO3−RR电催化剂提供了机会。
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来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
期刊介绍: The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.
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