單原子催化的理論基礎(chǔ)

李 雋*

清華大學(xué)化學(xué)系，理論化學(xué)中心，北京

*郵箱: junli@tsinghua.edu.cn

 

催化科學(xué)與技術(shù)對化學(xué)工業(yè)、生物轉(zhuǎn)化、大氣過程、環(huán)境保護(hù)、能源開發(fā)及人類健康等領(lǐng)域均具有重要作用。傳統(tǒng)的催化劑研發(fā)長期以來依賴反復(fù)試錯的實驗方法，這就迫切要求我們從本質(zhì)上理解催化反應(yīng)的活性位點與微觀作用機(jī)制。2011年張濤、李雋、劉景月提出單原子催化（single-atom catalysis）概念后^[1-3]，多相單原子催化劑（single-atom catalysts, SACs）與單團(tuán)簇催化劑（single-cluster catalysts, SCCs）近年來在催化領(lǐng)域引發(fā)了廣泛的研究興趣。這類新型催化劑擁有結(jié)構(gòu)明確、原子級精準(zhǔn)的活性位點，為多相催化反應(yīng)的高效調(diào)控理性設(shè)計提供了可能^[4,5]。本次報告將闡述基于單原子催化劑和單團(tuán)簇催化劑的原子級精準(zhǔn)多相催化（atomically precise heterogeneous catalysis, APCat）研究現(xiàn)狀與展望，探討單原子催化劑和單團(tuán)簇催化劑穩(wěn)定性與反應(yīng)性的理論基礎(chǔ)，并重點介紹其在重要的熱催化、電催化與光催化反應(yīng)中的潛在應(yīng)用。

 

參考文獻(xiàn)

[1] (a) B. Qiao, A. Wang, X. Yang, L. F. Allard, Z. Jiang, Y. Cui, J. Liu, J. Li, T. Zhang, Nat. Chem. 3: 634−641(2011). (b) X. Yang, A. Wang, B. Qiao, J. Li, J. Liu, T. Zhang, Acc. Chem. Res. 46: 1740-1748(2013). (c) A. Wang, J. Li, T. Zhang, Nat. Rev. Chem. 2: 65-81(2018).

[2] (a) J.-C. Liu, Y.-G. Wang, J. Li, J. Am. Chem. Soc. 139: 6190-6199 (2017). (b) J.-C. Liu, Y. Tang, Y.-G. Wang, T. Zhang, J. Li, Natl. Sci. Rev. 5: 638-641(2018).

[3] (a) X.-L. Ma, J.-C. Liu, H. Xiao, J. Li, J. Am. Chem. Soc. 140: 46-49(2018). (b) J.-C. Liu, X.-L. Ma, Y. Li, Y.-G. Wang, H. Xiao, J. Li, Nat. Commun. 9: 1610(2018). (c) X. Li, S. Mitchell, Y. Fang, J. Li, J. Perez-Ramirez, J. Lu, Nat. Rev. Chem. 7: 754–767(2023).

[4] (a) J.-C. Liu, J. Li, et al. CCS Chem. 5: 152-163(2023). (b) J.-X. Kang, Z. Yao, Z.-H. Wang, C.-Q. Xu, Y.-F. Jiang, Y.-G. Wang, X. Chen, J. Li, J. Chem. Phys. 164: 054703 (2026).

[5] (a) X. Hai, Y. Zheng, Q. Yu, J. Li, J. Lv, et al., Nature 622: 754–760(2023). (b) J. Ding, H. B. Yang, X.-L. Ma J. Li, B. Liu, et al., Nat. Energy 8:1386-1394(2023). (c) Y. Guo, J.-X. Liang, Y. Huang, J. Yang, Q. Zhang, A. Wang, B. Qiao, J. Li, T. Zhang, Acc. Chem. Res. 58: 2440-2453(2025).

 

Theoretical Foundations of Single-Atom Catalysis

Jun Li (李 雋)*

Theoretical Chemistry Center, Department of Chemistry, Tsinghua University, *Email: junli@tsinghua.edu.cn 

 

maximum Catalysis science and technology have played a key role in chemical industries, biological transformation, atmospheric processes, environment, energy, and human health. Conventionally, catalysts are discovered based on trial-and-error experiments, which calls for rational understanding of the active sites and microscopic mechanisms of catalytic reactions. In recent years, heterogeneous single-atom catalysts (SACs) and single-cluster catalysts (SCCs) have aroused significant interest in the catalysis community since we created the concept of single-atom catalysis in 2011[1-3]. These new types of catalysts offer well-defined atomically precise active sites that enable manipulation and design of heterogeneous catalytic reactions [4,5]. In this talk, we will provide an overview and perspective of atomically precise heterogeneous catalysis (APCat) via SACs and SCCs. The theoretical foundations of the stability and reactivity of SACs and SCCs will be discussed. Possible applications in thermo-, electro- and photo-catalysis of critical catalytic reactions will be highlighted.

 

References

[1] (a) B. Qiao, A. Wang, X. Yang, L. F. Allard, Z. Jiang, Y. Cui, J. Liu, J. Li, T. Zhang, Nat. Chem. 3: 634−641(2011). (b) X. Yang, A. Wang, B. Qiao, J. Li, J. Liu, T. Zhang, Acc. Chem. Res. 46: 1740-1748(2013). (c) A. Wang, J. Li, T. Zhang, Nat. Rev. Chem. 2: 65-81(2018).

[2] (a) J.-C. Liu, Y.-G. Wang, J. Li, J. Am. Chem. Soc. 139: 6190-6199 (2017). (b) J.-C. Liu, Y. Tang, Y.-G. Wang, T. Zhang, J. Li, Natl. Sci. Rev. 5: 638-641(2018).

[3] (a) X.-L. Ma, J.-C. Liu, H. Xiao, J. Li, J. Am. Chem. Soc. 140: 46-49(2018). (b) J.-C. Liu, X.-L. Ma, Y. Li, Y.-G. Wang, H. Xiao, J. Li, Nat. Commun. 9: 1610(2018). (c) X. Li, S. Mitchell, Y. Fang, J. Li, J. Perez-Ramirez, J. Lu, Nat. Rev. Chem. 7: 754–767(2023).

[4] (a) J.-C. Liu, J. Li, et al. CCS Chem. 5: 152-163(2023). (b) J.-X. Kang, Z. Yao, Z.-H. Wang, C.-Q. Xu, Y.-F. Jiang, Y.-G. Wang, X. Chen, J. Li, J. Chem. Phys. 164: 054703 (2026).

[5] (a) X. Hai, Y. Zheng, Q. Yu, J. Li, J. Lv, et al., Nature 622: 754–760(2023). (b) J. Ding, H. B. Yang, X.-L. Ma J. Li, B. Liu, et al., Nat. Energy 8:1386-1394(2023). (c) Y. Guo, J.-X. Liang, Y. Huang, J. Yang, Q. Zhang, A. Wang, B. Qiao, J. Li, T. Zhang, Acc. Chem. Res. 58: 2440-2453(2025).

 

李 雋，清華大學(xué)化學(xué)系教授, 理論化學(xué)中心主任。1992年在中國科學(xué)院福建物質(zhì)結(jié)構(gòu)研究所獲博士學(xué)位，師從我國著名化學(xué)家盧嘉錫院士。1994-1997年在德國和美國從事博士后研究工作，1997-2007年先后擔(dān)任Ohio州立大學(xué)研究科學(xué)家、美國西北太平洋國家實驗室高級研究科學(xué)家和資深科學(xué)家。

2004年入選清華大學(xué)百人計劃，被聘為化學(xué)系教授、博士生導(dǎo)師，并受聘為教育部長江學(xué)者特聘教授，2005年獲國家杰出青年科學(xué)基金資助。2010年獲選為美國科學(xué)促進(jìn)會會士(AAAS Fellow)，2018年獲國家自然科學(xué)二等獎, 2020年獲選為中國化學(xué)會會士，2025年當(dāng)選為中國科學(xué)院院士。長期從事鑭系錒系理論化學(xué)和計算催化等領(lǐng)域的研究工作。目前在SCI雜志上發(fā)表論文600余篇，其中在國際頂級雜志(Science, PNAS, Nature及其子刊, JACS, Angew. Chem., Acc. Chem. Res. )上發(fā)表論文170 余篇，論文引用7.5萬次。