Effects of the chemical states of N sites and mesoporosity of N-doped carbon supports on single-atom Ru catalysts during CO2-to-formate conversion

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2024-01-18 DOI:10.1016/j.apcatb.2024.123751

Kwangho Park , Kyung Rok Lee , Sunghee Ahn , Canh Van Nguyen , Kwang-Deog Jung

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Abstract

This study explores the fabrication and characterization of mesoporous nitrogen-doped carbon replicas (MNCs) as Ru catalyst supports for CO₂ hydrogenation to formate. MNC supports with a cubic Ia3d-like structure were successfully synthesized from a KIT-6 template. The mesoporosity, N content, and N states in the MNCs differed according to the precursor type, which substantially influenced the stability of single-atom Ru catalysts during CO₂ conversion. In hydrogenation tests, the Ru/MNC prepared using acrylonitrile precursor (Ru/MNC-A) demonstrated the best stability, whereas the Ru/MNCs prepared using pyrrole and melamine exhibited low activity owing to Ru agglomeration and limited reactant diffusion, respectively. The excellent stability of Ru/MNC-A resulted from Ru migration and rearrangement, as evidenced by near edge X-ray absorption fine structure analyses. Ru/MNC-A and Ru/MNC-A-400 achieved an outstanding turnover number of 69,000 in CO₂ hydrogenation over 72 h. Remarkably, the Ru/MNC-A catalyst demonstrated exceptional stability, attaining a TON of 315,840 over 360 h.

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二氧化碳转化为甲酸盐过程中 N 位点的化学状态和掺杂 N 的碳载体的介孔率对单原子 Ru 催化剂的影响

本研究探讨了作为 Ru 催化剂载体的介孔掺氮复型碳（MNCs）的制备和表征，用于 CO2 加氢制甲酸盐。利用 KIT-6 模板成功合成了具有类似立方 Ia3d 结构的 MNC 支撑物。根据前驱体类型的不同，MNCs 中的介孔率、N 含量和 N 状态也不同，这在很大程度上影响了单原子 Ru 催化剂在 CO2 转化过程中的稳定性。在氢化测试中，使用丙烯腈前驱体制备的 Ru/MNC （Ru/MNC-A）表现出最佳稳定性，而使用吡咯和三聚氰胺制备的 Ru/MNC 则分别由于 Ru 团聚和反应物扩散受限而表现出低活性。近边缘 X 射线吸收精细结构分析表明，Ru/MNC-A 的优异稳定性源于 Ru 的迁移和重排。Ru/MNC-A 和 Ru/MNC-A-400 在 72 小时的二氧化碳加氢过程中实现了 69,000 的出色周转次数。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.