Facilely tunable dodecahedral polyoxometalate framework loaded with mono- or bimetallic sites for efficient photocatalytic CO2 reduction

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2024-01-14 DOI:10.1016/j.apcatb.2024.123733

Bonan Li , Mengxue Chen , Qiyu Hu , Jiayu Zhu , Xu Yang , Zhexu Li , Chunlian Hu , Yuanyuan Li , Ping Ni , Yong Ding

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Abstract

Utilizing solar energy to drive the conversion of CO₂ into high-value chemicals emerged as a promising approach to decrease CO₂ emission. Yolk-shell or hollow structure have drawn much attention for photocatalytic CO₂ reduction, owing to their efficient CO₂ trapping and more active sites exposing. In this study, we employed a simple method to regulate the morphological evolution of K₃PW₁₂O₄₀ dodecahedra. After annealing, mono-/bimetallic active species are homogeneously dispersed on K₃PW₁₂O₄₀ framework forming PW₁₂ @Co and PW₁₂ @CoNi, which exhibit good CO production rates of 11.2 and 15.1 μmol/h, respectively, with selectivity of 90.7% and 92.6%. The differences in the activity and selectivity of CO₂RR are attributed to the morphology variations of POM and the influence of mono-/bimetallic species. These results are confirmed through the analysis of SEM, TEM, N₂ and CO₂ adsorption/desorption, PL, EIS and SPV characterizations. In-situ DRIFTS and DFT provide further support for the formation and transformation of intermediate products.

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十二面体 POM 框架负载单金属或双金属位点，可轻松调谐，用于高效光催化还原 CO2

利用太阳能将二氧化碳转化为高价值的化学物质，已成为减少二氧化碳排放的一种前景广阔的方法。卵壳或空心结构因其高效的二氧化碳捕集和更多的活性位点暴露，在光催化还原二氧化碳方面备受关注。在本研究中，我们采用了一种简单的方法来调节 K3PW12O40 十二面体的形态演变。退火后，单/双金属活性物种均匀地分散在 K3PW12O40 框架上，形成 PW12@Co 和 PW12@CoNi，它们表现出良好的 CO 生成率，分别为 11.2 和 15.1 μmol/h，选择性分别为 90.7% 和 92.6%。CO2RR 活性和选择性的差异归因于 POM 的形态变化以及单/双金属物种的影响。这些结果通过 SEM、TEM、N2 和 CO2 吸附/解吸、PL、EIS 和 SPV 表征分析得到了证实。原位 DRIFTS 和 DFT 为中间产物的形成和转化提供了进一步的支持。

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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.