Highly Active Photoreduction of Atmospheric-Concentration CO2 into CH3COOH over Palladium Particles on Nb2O5 Nanosheets

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2024-09-18 DOI:10.1002/anie.202414453
Jinyu Ding, Peijin Du, Peipei Li, Wenxiu Liu, Jiaqi Xu, Wensheng Yan, Yang Pan, Jun Hu, Junfa Zhu, Qingxia Chen, Xingchen Jiao, Yie Xie
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Abstract

The endeavor to drive CO2 photoreduction towards the synthesis of C2 products is largely thwarted by the colossal energy hurdle inherent in C−C coupling. Herein, we load active metal particles on metal oxide nanosheets to build the dual metal pair sites for steering C−C coupling to form C2 products. Taking Pd particles anchored on the Nb2O5 nanosheets as an example, the high-angle annular dark-field image and X-ray photoelectron spectroscopy demonstrate the presence of Pd−Nb metal pair sites on the Pd-Nb2O5 nanosheets. Density functional theory calculations reveal these sites exhibit a low reaction energy barrier of only 1.02 eV for C−C coupling, implying that the introduction of Pd particles effectively tailors the reaction step to form C2 products. Therefore, the Pd-Nb2O5 nanosheets achieve a CH3COOH evolution rate of 13.5 μmol g−1 h−1 in photoreduction of atmospheric-concentration CO2, outshining all other single photocatalysts reported to date under analogous conditions.
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Nb2O5 纳米片上的钯粒子将大气浓度的 CO2 高活性光还原成 CH3COOH
C-C耦合固有的巨大能量障碍在很大程度上阻碍了推动二氧化碳光还原合成 C2 产物的努力。在此,我们在金属氧化物纳米片上装载活性金属颗粒,以建立双金属对位点,引导 C-C 耦合形成 C2 产物。以锚定在 Nb2O5 纳米片上的 Pd 粒子为例,高角度环形暗场图像和 X 射线光电子能谱显示 Pd-Nb2O5 纳米片上存在 Pd-Nb 金属对位点。密度泛函理论计算显示,这些位点在 C-C 耦合过程中表现出较低的反应能垒,仅为 1.02 eV,这意味着钯粒子的引入能有效地调整反应步骤,形成 C2 产物。因此,Pd-Nb2O5 纳米片在光还原大气浓度 CO2 的过程中,CH3COOH 的进化速率达到了 13.5 μmol g-1 h-1,超过了迄今为止在类似条件下报道的所有其他单一光催化剂。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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