Electronic interaction between transition metal single-atoms and anatase TiO2 boosts CO2 photoreduction with H2O,Energy & Environmental Science

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Electronic interaction between transition metal single-atoms and anatase TiO2 boosts CO2 photoreduction with H2O
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2021-09-20 , DOI: 10.1039/d1ee01574e
Byoung-Hoon Lee _{1,

2} , Eunhee Gong ₃ , Minho Kim _{4,

5} , Sunghak Park ₆ , Hye Rim Kim ₃ , Junho Lee ₃ , Euiyeon Jung _{1,

2} , Chan Woo Lee _{1,

2} , Jinsol Bok _{1,

2} , Yoon Jung _{1,

2} , Young Seong Kim ₁ , Kug-Seung Lee ₇ , Sung-Pyo Cho ₈ , Jin-Woo Jung ₉ , Chang-Hee Cho ₉ , Sébastien Lebègue ₄ , Ki Tae Nam ₆ , Hyungjun Kim ₁₀ , Su-Il In ₃ , Taeghwan Hyeon _{1,

2}

Affiliation

Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea
School of Chemical and Biological Engineering, and Institute of Chemical Processes, Seoul National University, Seoul 08826, Republic of Korea
Department of Energy Science & Engineering, Daegu Gyeongbuk Institute of Science and Technology (DGIST), Daegu, 42988, Republic of Korea
Université de Lorraine and CNRS, LPCT, UMR 7019, Vandœuvre-lès-Nancy 54506, France
Department of Applied Chemistry, Kyung Hee University, Yongin, Gyeonggi 17104, Republic of Korea
Department of Materials Science and Engineering, Seoul National University, Seoul 08826, Republic of Korea
Pohang Accelerator Laboratory (PAL), Pohang University of Science and Technology (POSTECH), Pohang 37673, Republic of Korea
National Center for Inter-University Research Facilities, Seoul National University, Seoul 08826, Republic of Korea
Department of Emerging Materials Science, DGIST, Daegu 42988, South Korea
Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea

Single-atom catalysts are playing a pivotal-role in understanding atomic-level photocatalytic processes. However, single-atoms are typically non-uniformly distributed on photocatalyst surfaces, hindering the systematic investigation of structure–property correlation at atomic precision. Herein, by combining material design, spectroscopic analyses, and theoretical studies, we investigate the atomic-level CO₂ photoreduction process on TiO₂ photocatalysts with uniformly stabilized transition metal single-atoms. First, the electronic interaction between single Cu atoms and the surrounding TiO₂ affects the reducibility of the TiO₂ surface, leading to spontaneous O vacancy formation near Cu atoms. The coexistence of Cu atoms and O vacancies cooperatively stabilizes CO₂ intermediates on the TiO₂ surface. Second, our approach allows us to control the spatial distribution of uniform single Cu atoms on TiO₂, and demonstrate that neighboring Cu atoms simultaneously engage in the interaction with CO₂ intermediates by controlling the charge localization. Optimized Cu₁/TiO₂ photocatalysts exhibit 66-fold enhancement in CO₂ photoreduction performance compared to the pristine TiO₂.

中文翻译：

过渡金属单原子和锐钛矿 TiO2 之间的电子相互作用促进了 H2O 对 CO2 的光还原

单原子催化剂在理解原子级光催化过程中发挥着关键作用。然而，单原子通常不均匀地分布在光催化剂表面，阻碍了以原子精度进行结构-性质相关性的系统研究。这里，通过组合的材料设计，光谱的分析，和理论研究，我们调查原子级CO ₂光还原过程在TiO _2层的光催化剂与均匀地稳定过渡金属的单原子。首先，单一Cu原子与周围的TiO之间的电子相互作用₂影响TiO 2的还原₂表面，导致在 Cu 原子附近自发形成 O 空位。Cu原子和O空位的共存协同稳定了TiO ₂表面上的CO ₂中间体。其次，我们的方法允许我们控制 TiO ₂上均匀单个 Cu 原子的空间分布，并证明相邻的 Cu 原子通过控制电荷定位同时参与与 CO ₂中间体的相互作用。与原始的 TiO ₂相比，优化的 Cu ₁ /TiO ₂光催化剂在 CO _{2 光}还原性能方面表现出 66 倍的增强。

更新日期：2021-09-20

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