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引用次数: 0
摘要
催化性能通常对催化剂表面的纳米级和原子级结构非常敏感,而影响中观尺度物种迁移的关键因素却往往被忽视。在此,我们利用具有可调平均粒子间距的模型铜纳米粒子气体扩散电极,揭示了粒子间距在工业相关电流密度下调整 CO 电解产物选择性中的作用。增加纳米铜粒子的平均粒子间距可显著提高对醋酸盐(一种特定的多碳产物)的选择性。实验和数值计算结果表明,粒子间距越大,Cu 纳米粒子附近的局部 pH 值和局部 CO 浓度就越高,这是由于粒子间的 CO 扩散在中尺度上减弱了。通过耦合外部反应条件,最大醋酸法拉第效率和部分电流密度分别达到 77.5% 和 705 mA cm-2。我们的研究结果表明,在工业相关条件下的复杂催化反应中,作为介观描述因子的粒子间距离对于选择性控制非常重要。
Interparticle Distance Matters for Selectivity Control in Industrially Relevant CO Electrolysis
While catalytic performances are usually sensitive to catalyst surface structures at the nanoscale and atomic scale, crucial factors affecting species transport at the mesoscale are often overlooked. Here we reveal the role of interparticle distance in tuning product selectivity in CO electrolysis at industrially relevant current densities using model Cu nanoparticle gas diffusion electrodes with tunable average interparticle distances. Increasing the average interparticle distance of Cu nanoparticles remarkably increases the selectivity toward acetate, a specific multicarbon product. Experimental and numerical calculation results indicate that a larger interparticle distance increases the local pH near Cu nanoparticles and the local CO concentration owing to weakened interparticle CO diffusion at the mesoscale. By coupling external reaction conditions, the maximum acetate Faradaic efficiency and partial current density reach 77.5% and 705 mA cm–2, respectively. Our findings illustrate the importance of interparticle distance as a mesoscopic descriptor for selectivity control in complex catalytic reactions under industrially relevant conditions.
ACS Energy Letters Energy-Renewable Energy, Sustainability and the Environment
CiteScore
31.20
自引率
5.00%
发文量
469
审稿时长
1 months
期刊介绍:
ACS Energy Letters is a monthly journal that publishes papers reporting new scientific advances in energy research. The journal focuses on topics that are of interest to scientists working in the fundamental and applied sciences. Rapid publication is a central criterion for acceptance, and the journal is known for its quick publication times, with an average of 4-6 weeks from submission to web publication in As Soon As Publishable format.
ACS Energy Letters is ranked as the number one journal in the Web of Science Electrochemistry category. It also ranks within the top 10 journals for Physical Chemistry, Energy & Fuels, and Nanoscience & Nanotechnology.
The journal offers several types of articles, including Letters, Energy Express, Perspectives, Reviews, Editorials, Viewpoints and Energy Focus. Additionally, authors have the option to submit videos that summarize or support the information presented in a Perspective or Review article, which can be highlighted on the journal's website. ACS Energy Letters is abstracted and indexed in Chemical Abstracts Service/SciFinder, EBSCO-summon, PubMed, Web of Science, Scopus and Portico.