{"title":"Isolated Ni Atoms Enable Near-Unity CH<sub>4</sub> Selectivity for Photothermal CO<sub>2</sub> Hydrogenation.","authors":"Fazal Raziq, Chengyang Feng, Miao Hu, Shouwei Zuo, Mohammad Ziaur Rahman, Yayu Yan, Qiao-Hong Li, Jorge Gascon, Huabin Zhang","doi":"10.1021/jacs.4c05873","DOIUrl":null,"url":null,"abstract":"<p><p>Photothermal hydrogenation of carbon dioxide (CO<sub>2</sub>) into value-added products is an ideal solution for addressing the energy crisis and mitigating CO<sub>2</sub> emissions. However, achieving high product selectivity remains challenging due to the simultaneous occurrence of numerous competing intermediate reactions during CO<sub>2</sub> hydrogenation. We present a novel approach featuring isolated single-atom nickel (Ni) anchored onto indium oxide (In<sub>2</sub>O<sub>3</sub>) nanocrystals, serving as an effective photothermal catalyst for CO<sub>2</sub> hydrogenation into methane (CH<sub>4</sub>) with a remarkable near-unity (∼99%) selectivity. Experiments and theoretical simulations have confirmed that isolated Ni sites on the In<sub>2</sub>O<sub>3</sub> surface can effectively stabilize the intermediate products of the CO<sub>2</sub> hydrogenation reaction and reduce the transition state energy barrier, thereby changing the reaction path to achieve ultrahigh selective methanation. This study provides comprehensive insights into the design of single-atom catalysts for the highly selective photothermal catalytic hydrogenation of CO<sub>2</sub> to methane.</p>","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":null,"pages":null},"PeriodicalIF":14.4000,"publicationDate":"2024-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jacs.4c05873","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/6/13 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Photothermal hydrogenation of carbon dioxide (CO2) into value-added products is an ideal solution for addressing the energy crisis and mitigating CO2 emissions. However, achieving high product selectivity remains challenging due to the simultaneous occurrence of numerous competing intermediate reactions during CO2 hydrogenation. We present a novel approach featuring isolated single-atom nickel (Ni) anchored onto indium oxide (In2O3) nanocrystals, serving as an effective photothermal catalyst for CO2 hydrogenation into methane (CH4) with a remarkable near-unity (∼99%) selectivity. Experiments and theoretical simulations have confirmed that isolated Ni sites on the In2O3 surface can effectively stabilize the intermediate products of the CO2 hydrogenation reaction and reduce the transition state energy barrier, thereby changing the reaction path to achieve ultrahigh selective methanation. This study provides comprehensive insights into the design of single-atom catalysts for the highly selective photothermal catalytic hydrogenation of CO2 to methane.
光热氢化将二氧化碳(CO2)转化为高附加值产品是解决能源危机和减少二氧化碳排放的理想方案。然而,由于二氧化碳氢化过程中会同时发生许多相互竞争的中间反应,因此实现高产品选择性仍具有挑战性。我们提出了一种新方法,将孤立的单原子镍(Ni)锚定在氧化铟(In2O3)纳米晶体上,作为一种有效的光热催化剂,将 CO2 加氢转化为甲烷(CH4),具有显著的近乎统一(∼99%)的选择性。实验和理论模拟证实,In2O3 表面孤立的 Ni 位点能有效稳定 CO2 加氢反应的中间产物,降低过渡态能垒,从而改变反应路径,实现超高选择性甲烷化。这项研究为设计用于高选择性光热催化 CO2 加氢制甲烷的单原子催化剂提供了全面的见解。
期刊介绍:
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