Single-atom Pt–N4 active sites anchored on porous C3N4 nanosheet for boosting the photocatalytic CO2 reduction with nearly 100% CO selectivity

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2024-01-15 DOI:10.1016/j.apcatb.2024.123737

Shan Hu , Panzhe Qiao , Xinming Liang , Guiming Ba , Xiaolong Zu , Huilin Hu , Jinhua Ye , Defa Wang

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Abstract

Photoreduction of CO₂ and H₂O into fuels and value-added chemicals is a promising green technology for solar-to-chemical conversion. However, improving the conversion efficiency with regulated product selectivity is a big challenge due to the sluggish dynamic transfer and insufficient active sites. Herein, we report on Pt single atoms anchored porous C₃N₄ nanosheet photocatalyst (Pt₁@CN) with Pt–N₄ coordination for stable and efficient CO₂ photoreduction using H₂O as reductant. The Pt₁@CN exhibits an evolution rate of 84.8 μmol g⁻¹ h⁻¹ with nearly 100% CO selectivity, outperforming most previous C₃N₄-based single-atom photocatalysts. Experimental and DFT calculation results reveal that the Pt–N₄ coordinated active sites promote the photogenerated electron transfer, CO₂ adsorption/activation, *COOH generation, and *CO desorption, thus accounting for the significantly improved CO₂ photoreduction activity with ∼100% CO selectivity. This study provides a deep insight into the significant roles of single-atom active sites in enhancing the CO₂ photoreduction activity and regulating the product selectivity.

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在多孔 C3N4 纳米片上锚定单原子 Pt-N4 活性位点，以接近 100% 的 CO 选择性提高光催化 CO2 还原效率

将 CO2 和 H2O 光还原成燃料和高附加值化学品是一项前景广阔的太阳能转化为化学品的绿色技术。然而，由于动态转移迟缓和活性位点不足，在调节产品选择性的同时提高转化效率是一项巨大挑战。在此，我们报告了锚定铂单原子的多孔 C3N4 纳米片状光催化剂（Pt1@CN），该催化剂具有 Pt-N4 配位，能以 H2O 为还原剂稳定高效地进行 CO2 光还原。Pt1@CN 的进化速率为 84.8 μmol g-1 h-1，CO 选择性接近 100%，优于之前大多数基于 C3N4 的单原子光催化剂。实验和 DFT 计算结果表明，Pt-N4 配位活性位点促进了光生电子转移、CO2 吸附/活化、*COOH 生成和*CO 解吸，从而显著提高了 CO2 光还原活性，CO 选择性高达 100%。这项研究深入揭示了单原子活性位点在提高 CO2 光还原活性和调节产物选择性方面的重要作用。

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

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.