Boosting selective chlorine evolution reaction: Impact of Ag doping in RuO2 electrocatalysts

IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL
Yinlong Cheng , Pengyu Meng , Liansheng Li , Lixiang Zhong , Chengzong Yuan , Jie Chen , Qinghua Liang
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Abstract

The chlor-alkali process is critical to the modern chemical industry because of the wide utilization of chlorine gas (Cl2). More than 95 % of global Cl2 production relies on electrocatalytic chlorine evolution reaction (CER) through chlor-alkali electrolysis. The RuO2 electrocatalyst serves as the main active component widely used in commercial applications. However, oxygen evolution reaction (OER) generally competes with CER electrocatalysts at RuO2 electrocatalyst owing to the intrinsically scaling reaction energy barrier of *OCl and *OOH intermediates, leading to decreased CER selectivity, high energy consumption, and increased cost. Here, the effect of Ag doping on selective CER over RuO2 electrocatalysts prepared by a sol–gel method has been systematically studied. We found that Ag-doping can effectively improve the Faradaic efficiency of RuO2 electrocatalyst for CER. Furthermore, the improved CER selectivity of Ag-doped RuO2 electrocatalysts is highly dependent on the Ag-doping concentration. The optimized Ag0.15Ru0.85O2 electrocatalyst displays an overpotential of 105 mV along with a selectivity of 84.64 ± 1.84 % in 5.0 M NaCl electrolyte (pH = 2.0 ± 0.05), significantly outperforming undoped one (142 mV, 72.75 ± 1.52 %). Our experiments and density functional theory (DFT) calculations show electron transfer from Ag+ to Ru4+ suppresses *OOH intermediates desorption on Ag-doped RuO2, enabling improved CER selectivity. Such designs of Ag-doped RuO2 electrocatalysts are expected to be favorable for practical chlor-alkali applications.

Abstract Image

促进选择性析氯反应:Ag掺杂对RuO2电催化剂的影响。
由于氯气(Cl2)的广泛利用,氯碱工艺对现代化工至关重要。全球95%以上的Cl2生产依赖于氯碱电解电催化析氯反应(CER)。RuO2电催化剂是广泛应用于商业应用的主要活性组分。然而,由于*OCl和*OOH中间体固有的结垢反应能垒,OER通常在RuO2电催化剂上与CER电催化剂竞争,导致CER选择性降低,能耗高,成本增加。本文系统地研究了Ag掺杂对溶胶-凝胶法制备的RuO2电催化剂选择性CER的影响。我们发现ag掺杂可以有效地提高RuO2电催化剂的法拉第效率。此外,ag掺杂的RuO2电催化剂的CER选择性的提高高度依赖于ag掺杂浓度。优化后的Ag0.15Ru0.85O2电催化剂在5.0 M NaCl电解液(pH = 2.0±0.05)中的过电位为105 mV,选择性为84.64±1.84%,显著优于未掺杂的Ag0.15Ru0.85O2电催化剂(142 mV, 72.75±1.52%)。我们的实验和密度泛函理论(DFT)计算表明,从Ag+到Ru4+的电子转移抑制了*OOH中间体在Ag掺杂的RuO2上的解吸,从而提高了CER选择性。这种设计的ag掺杂的RuO2电催化剂有望有利于氯碱的实际应用。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
CiteScore
16.10
自引率
7.10%
发文量
2568
审稿时长
2 months
期刊介绍: The Journal of Colloid and Interface Science publishes original research findings on the fundamental principles of colloid and interface science, as well as innovative applications in various fields. The criteria for publication include impact, quality, novelty, and originality. Emphasis: The journal emphasizes fundamental scientific innovation within the following categories: A.Colloidal Materials and Nanomaterials B.Soft Colloidal and Self-Assembly Systems C.Adsorption, Catalysis, and Electrochemistry D.Interfacial Processes, Capillarity, and Wetting E.Biomaterials and Nanomedicine F.Energy Conversion and Storage, and Environmental Technologies
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