WO3-TiO2负载的Pt单原子催化剂光热协同催化丙烷和丙烯氧化

doi:10.3866/PKU.WHXB202303003

物理化学学报 >> 2024, Vol. 40 >> Issue (1): 2303003.doi: 10.3866/PKU.WHXB202303003

所属专题：多物理场能源催化转化

WO₃-TiO₂负载的Pt单原子催化剂光热协同催化丙烷和丙烯氧化

朱锐杰¹^,², 康磊磊¹, 李林¹, 潘晓丽¹, 王华¹, 苏杨¹, 李广亿¹, 程鸿魁³, 李仁贵⁴^,⁵, 刘晓艳¹^,⁴^,*(), 王爱琴¹^,²

¹ 中国科学院大连化学物理研究所, 中国科学院航天催化材料重点实验室, 能源材料化学协同创新中心, 辽宁大连 116023
² 中国科学院大学, 北京 100049
³ 正大能源材料(大连)有限公司, 辽宁大连 116021
⁴ 中国科学院大连化学物理研究所, 催化基础国家重点实验室, 辽宁大连 116023
⁵ 大连洁净能源国家实验室, 辽宁大连 116023

收稿日期:2023-03-01 录用日期:2023-04-10 发布日期:2023-08-21
通讯作者: 刘晓艳 E-mail:xyliu2003@dicp.ac.cn
作者简介:第一联系人：
^†These authors contributed equally to this work.
基金资助:
国家自然科学基金(22102180);辽宁省兴辽英才计划(XLYC2007070);中国科学院洁净能源创新研究院合作基金(DNL202002);中央高校基本科研业务费专项资金(20720220009)

Photo-Thermo Catalytic Oxidation of C₃H₈ and C₃H₆ over the WO₃-TiO₂ Supported Pt Single-Atom Catalyst

Ruijie Zhu¹^,², Leilei Kang¹, Lin Li¹, Xiaoli Pan¹, Hua Wang¹, Yang Su¹, Guangyi Li¹, Hongkui Cheng³, Rengui Li⁴^,⁵, Xiao Yan Liu¹^,⁴^,*(), Aiqin Wang¹^,²

¹ Dalian Institute of Chemical Physics, CAS Key Laboratory of Science and Technology on Applied Catalysis, iChEM, Chinese Academy of Sciences, Dalian 116023, Liaoning Province, China
² University of Chinese Academy of Sciences, Beijing 100049, China
³ Chia Tai Energy Materials (Dalian) Co., Ltd., Dalian 116021, Liaoning Province, China
⁴ Dalian Institute of Chemical Physics, State Key Laboratory of Catalysis, Chinese Academy of Sciences, Dalian 116023, Liaoning Province, China
⁵ Dalian National Laboratory for Clean Energy, Dalian 116023, Liaoning Province, China

Received:2023-03-01 Accepted:2023-04-10 Published:2023-08-21
Contact: Xiao Yan Liu E-mail:xyliu2003@dicp.ac.cn
Supported by:
the National Natural Science Foundation of China(22102180);the Liaoning Revitalization Talents Program, China(XLYC2007070);the Dalian National Laboratory Cooperation Fund, Chinese Academy of Sciences(DNL202002);the Fundamental Research Funds for the Central Universities, China(20720220009)

1. WHXB202303003-SI-7p.pdf(1631KB)

摘要/Abstract

摘要：

单原子催化剂(single-atom catalyst，SAC)可以最大化金属原子利用率，并具有独特的电子特性，已经在各种催化反应中进行了广泛的探索。然而，与纳米催化剂相比，贵金属SAC在烃类氧化反应中通常被认为是不活泼的。在本文中，证明了WO₃-TiO₂负载的Pt SAC (Pt₁/WO₃-TiO₂)在光热协同催化氧化C₃H₈和C₃H₆这两种典型的挥发性有机化合物(VOCs)中表现出比相应的纳米催化剂(Pt_NP/WO₃-TiO₂)高得多的活性。研究发现，Pt₁/WO₃-TiO₂和Pt_NP/WO₃-TiO₂都可以通过克服氧中毒来提高光热协同催化C₃H₈氧化的活性。值得注意的是，Pt₁/WO₃-TiO₂的反应速率达到了3792 μmol∙g_Pt⁻¹∙s⁻¹，这对C₃H₈氧化是一个新的突破。更有趣的是，由于C₃H₆在Pt_NP/WO₃-TiO₂上的强吸附导致催化剂C₃H₆中毒，因此Pt_NP/WO₃-TiO₂上的光热协同催化C₃H₆氧化无法进行。但是，得益于C₃H₆和Pt单原子之间适中的相互作用，Pt₁/WO₃-TiO₂上的C₃H₆中毒在光照下可以被克服。因此，Pt₁/WO₃-TiO₂在光热协同催化C₃H₆氧化中显示出更高的活性。这项工作表明，SAC的优势不仅在于节约贵金属，还在于可以根据其独特的电子特性发现新的催化反应。

关键词: 单原子催化剂, 光热协同催化, 氧化反应, 氧中毒, 丙烯中毒

Abstract:

Catalytic oxidation is a commonly employed technology in the industry for removing volatile organic compounds (VOCs) due to its exceptional efficiency under mild operating conditions. Although supported Pt-based nano-catalysts are recognized widely as one of the most promising and extensively used industrial catalysts for VOC abatement, their practical application, and development are restricted by their exorbitant cost. Single-atom catalyst (SAC) with maximized metal utilization and exclusive electronic character has been explored extensively in various catalytic reactions. However, Pt SAC is usually deemed to be inactive in hydrocarbon oxidation reactions in thermal catalysis, compared with its nanoparticle counterpart. Here, we demonstrate that the WO₃-TiO₂ supported Pt SAC (Pt₁/WO₃-TiO₂) exhibits much higher activities than the corresponding nanoparticle catalyst (Pt_NP/WO₃-TiO₂) in photo-thermo catalytic oxidation of C₃H₈ and C₃H₆, which represent different kinds of typical VOCs. A key finding is that the activities of Pt₁/WO₃-TiO₂ and Pt_NP/WO₃-TiO₂ can be accelerated in photo-thermo catalytic C₃H₈ oxidation by overcoming oxygen poisoning. Upon the light irradiation, the apparent active energy (E_a) of the Pt₁/WO₃-TiO₂ and Pt_NP/WO₃-TiO₂ decline from 116 to 60 kJ·mol⁻¹ and from 103 to 30 kJ·mol⁻¹, respectively, substantiating their effectiveness in photo-thermo catalysis. Notably, a substantially higher reaction rate of 3792 μmol∙g_Pt⁻¹∙s⁻¹ on the Pt₁/WO₃-TiO₂ is achieved, which should be a benchmark for C₃H₈ oxidation. More intriguingly, photo-thermo catalytic C₃H₆ oxidation on the Pt_NP/WO₃-TiO₂ is prohibited due to the strong adsorption-induced C₃H₆ poisoning on the Pt nanoparticles, for which the E_a of the Pt_NP/WO₃-TiO₂ catalyst for C₃H₆ oxidation is maintained at approximately 55 kJ·mol⁻¹, regardless of the light irradiation. In comparison, the C₃H₆ poisoning on the Pt₁/WO₃-TiO₂ can be mitigated by light illumination, where the E_a of the Pt₁/WO₃-TiO₂ catalyst for C₃H₆ oxidation dramatically reduced from 49 to 16 kJ·mol⁻¹, signifying that the high energy barrier of C₃H₆ oxidation can be mediated by the light. Profiting from the apt affinity between C₃H₆ and Pt single atoms, the photogenerated electrons accumulated on the Pt single atoms produce repulsive force towards the electron-rich C₃H₆ molecules, which is conducive to the C₃H₆ desorption from the Pt₁/WO₃-TiO₂. Therefore, the Pt₁/WO₃-TiO₂ exhibits enhanced activity in photo-thermo catalytic C₃H₆ oxidation. This study exemplifies that the advantages of SAC are not only saving the consumption of precious metals but also discovering new catalytic reactions on the account of the specific electronic characteristic.

Key words: Single-atom catalyst, Photo-thermo catalysis, Oxidation reaction, Oxygen poisoning, Propylene poisoning

朱锐杰, 康磊磊, 李林, 潘晓丽, 王华, 苏杨, 李广亿, 程鸿魁, 李仁贵, 刘晓艳, 王爱琴. WO₃-TiO₂负载的Pt单原子催化剂光热协同催化丙烷和丙烯氧化[J]. 物理化学学报, 2024, 40(1), 2303003. doi: 10.3866/PKU.WHXB202303003

Ruijie Zhu, Leilei Kang, Lin Li, Xiaoli Pan, Hua Wang, Yang Su, Guangyi Li, Hongkui Cheng, Rengui Li, Xiao Yan Liu, Aiqin Wang. Photo-Thermo Catalytic Oxidation of C₃H₈ and C₃H₆ over the WO₃-TiO₂ Supported Pt Single-Atom Catalyst[J]. Acta Phys. -Chim. Sin. 2024, 40(1), 2303003. doi: 10.3866/PKU.WHXB202303003

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202303003

https://www.whxb.pku.edu.cn/CN/Y2024/V40/I1/2303003

图/表 5

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参考文献 46

1	Sadykov I. I. ; Zabilskiy M. ; Clark A. H. ; Krumeich F. ; Sushkevich V. ; van Bokhoven J. A. ; Nachtegaal M. ; Safonova O. V. ACS Catal. 2021, 11, 11793. doi: 10.1021/acscatal.1c02795
2	Chen G. ; Zhao Y. ; Fu G. ; Duchesne Paul N. ; Gu L. ; Zheng Y. ; Weng X. ; Chen M. ; Zhang P. ; Pao C. ; et al Science 2014, 344, 495. doi: 10.1126/science.1252553
3	Zhang B. ; Ren L. ; Xu Z. ; Cheng N. ; Lai W. ; Zhang L. ; Hao W. ; Chu S. ; Wang Y. ; Du Y. ; et al Small 2021, 17, 2100732. doi: 10.1002/smll.202100732
4	Chen C. ; Tian H. ; Fu Z. ; Cui X. ; Kong F. ; Meng G. ; Chen Y. ; Qi F. ; Chang Z. ; Zhu L. ; et al Appl. Catal. B 2022, 304, 121008. doi: 10.1016/j.apcatb.2021.121008
5	Shen R. ; Liu Y. ; Wen H. ; Wu X. ; Han G. ; Yue X. ; Mehdi S. ; Liu T. ; Cao H. ; Liang E. ; et al Small 2021, 18, 2105588. doi: 10.1002/smll.202105588
6	Đukić T. ; Moriau L. J. ; Pavko L. ; Kostelec M. ; Prokop M. ; Ruiz-Zepeda F. ; Šala M. ; Dražić G. ; Gatalo M. ; Hodnik N. ACS Catal. 2021, 12, 101. doi: 10.1021/acscatal.1c04205
7	Kato M. ; Iguchi Y. ; Li T. ; Kato Y. ; Zhuang Y. ; Higashi K. ; Uruga T. ; Saida T. ; Miyabayashi K. ; Yagi I. ACS Catal. 2021, 12, 259. doi: 10.1021/acscatal.1c04597
8	Zaman S. ; Su Y. ; Dong C. ; Qi R. ; Huang L. ; Qin Y. ; Huang Y. ; Li F. ; You B. ; Guo W. ; et al Angew. Chem. Int. Ed. 2022, 61, e202115835. doi: 10.1002/anie.202115835
9	Reina T. R. ; Gonzalez-Castaño M. ; Lopez-Flores V. ; Martínez T, L. M. ; Zitolo A. ; Ivanova S. ; Xu W. ; Centeno M. A. ; Rodriguez J. A. ; Odriozola J. A. J. Am. Chem. Soc. 2021, 144, 446. doi: 10.1021/jacs.1c10481
10	Zhai Y. ; Pierre D. ; Si R. ; Deng W. ; Ferrin P. ; Nilekar A. U. ; Peng G. ; Herron J. A. ; Bell D. C. ; Saltsburg H. ; et al Science 2010, 329, 1633. doi: 10.1126/science.1192449
11	Yang X. ; Wang A. ; Qiao B. ; Li J. ; Liu J. ; Zhang T. Acc. Chem. Res. 2013, 46, 1740. doi: 10.1021/ar300361m
12	Han B. ; Guo Y. ; Huang Y. ; Xi W. ; Xu J. ; Luo J. ; Qi H. ; Ren Y. ; Liu X. ; Qiao B. ; et al Angew. Chem. Int. Ed. 2020, 59, 11824. doi: 10.1002/anie.202003208
13	Kuo C. ; Lu Y. ; Kovarik L. ; Engelhard M. ; Karim A. M. ACS Catal. 2019, 9, 11030. doi: 10.1021/acscatal.9b02840
14	Li W. ; Yang J. ; Jing H. ; Zhang J. ; Wang Y. ; Li J. ; Zhao J. ; Wang D. ; Li Y. J. Am. Chem. Soc. 2021, 143, 15453. doi: 10.1021/jacs.1c08088
15	Wang L. ; Zhu C. ; Xu M. ; Zhao C. ; Gu J. ; Cao L. ; Zhang X. ; Sun Z. ; Wei S. ; Zhou W. ; et al J. Am. Chem. Soc. 2021, 143, 18854. doi: 10.1021/jacs.1c09498
16	Scirè S. ; Liotta L. F. Appl. Catal. B 2012, 125, 222. doi: 10.1016/j.apcatb.2012.05.047
17	FAO/FAOLEX OJEU 2004, L143, 87.
18	He C. ; Cheng J. ; Zhang X. ; Douthwaite M. ; Pattisson S. ; Hao Z. Chem. Rev. 2019, 119, 4471. doi: 10.1021/acs.chemrev.8b00408
19	Fang Y. ; Li H. ; Zhang Q. ; Wang C. ; Xu J. ; Shen H. ; Yang J. ; Pan C. ; Zhu Y. ; Luo Z. ; et al Environ. Sci. Technol. 2022, 56, 3245. doi: 10.1021/acs.est.1c07573
20	Zhang L. ; Xue L. ; Lin B. ; Zhao Q. ; Wan S. ; Wang Y. ; Jia H. ; Xiong H. ChemSusChem 2022, 15, e202102494. doi: 10.1002/cssc.202102494
21	Liu Y. ; Li X. ; Liao W. ; Jia A. ; Wang Y. ; Luo M. ; Lu J. ACS Catal. 2019, 9, 1472. doi: 10.1021/acscatal.8b03666
22	Yang A. ; Zhu H. ; Li Y. ; Cargnello M. ACS Catal. 2021, 11, 6672. doi: 10.1021/acscatal.1c01280
23	Kim J. ; Kim Y. ; Wiebenga M. H. ; Oh S. H. ; Kim D. H. Appl. Catal. B 2019, 251, 283. doi: 10.1016/j.apcatb.2019.04.001
24	Avgouropoulos G. ; Oikonomopoulos E. ; Kanistras D. ; Ioannides T. Appl. Catal. B 2006, 65, 62. doi: 10.1016/j.apcatb.2005.12.016
25	Yu X. ; He J. ; Wang D. ; Hu Y. ; Tian H. ; He Z. J. Phys. Chem. C 2012, 116, 851. doi: 10.1021/jp208947e
26	Zhang C. ; Liu F. ; Zhai Y. ; Ariga H. ; Yi N. ; Liu Y. ; Asakura K. ; Flytzani-Stephanopoulos M. ; He H. Angew. Chem. Int. Ed. 2012, 51, 9628. doi: 10.1002/anie.201202034
27	Jeong H. ; Lee G. ; Kim B. ; Bae J. ; Han J. W. ; Lee H. J. Am. Chem. Soc. 2018, 140, 9558. doi: 10.1021/jacs.8b04613
28	Jeong H. ; Kwon O. ; Kim B. ; Bae J. ; Shin S. ; Kim H. ; Kim J. ; Lee H. Nat. Catal. 2020, 3, 368. doi: 10.1038/s41929-020-0427-z
29	Wang Z. ; Song H. ; Liu H. ; Ye J. Angew. Chem. Int. Ed. 2020, 59, 8016. doi: 10.1002/anie.201907443
30	Christopher P. ; Xin H. ; Marimuthu A. ; Linic S. Nat. Mater. 2012, 11, 1044. doi: 10.1038/nmat3454
31	Tan T. H. ; Scott J. ; Ng Y. H. ; Taylor R. A. ; Aguey-Zinsou K.-F. ; Amal R. ACS Catal. 2016, 6, 1870. doi: 10.1021/acscatal.5b02785
32	Zhou L. ; Swearer D. F. ; Zhang C. ; Robatjazi H. ; Zhao H. ; Henderson L. ; Dong L. ; Christopher P. ; Carter E. A. ; Nordlander P. ; et al Science 2018, 362, 69. doi: 10.1126/science.aat6967
33	Kang L. ; Liu X. Y. ; Wang A. ; Li L. ; Ren Y. ; Li X. ; Pan X. ; Li Y. ; Zong X. ; Liu H. ; et al Angew. Chem. Int. Ed. 2020, 59, 12909. doi: 10.1002/anie.202001701
34	Feng Y. ; Dai L. ; Wang Z. ; Peng Y. ; Duan E. ; Liu Y. ; Jing L. ; Wang X. ; Rastegarpanah A. ; Dai H. ; et al Environ. Sci. Technol. 2022, 56, 8722. doi: 10.1021/acs.est.1c08643
35	Wang Y. ; Dai J. ; Wang M. ; Qi F. ; Jin X. ; Zhang L. J. Colloid Interface Sci. 2023, 636, 577. doi: 10.1016/j.jcis.2023.01.053
36	Lang R. ; Xi W. ; Liu J. ; Cui Y. ; Li T. ; Lee A. F. ; Chen F. ; Chen Y. ; Li L. ; Li L. ; et al Nat. Commun. 2019, 10, 234. doi: 10.1038/s41467-018-08136-3
37	DeRita L. ; Dai S. ; Lopez-Zepeda K. ; Pham N. ; Graham G. W. ; Pan X. ; Christopher P. J. Am. Chem. Soc. 2017, 139, 14150. doi: 10.1021/jacs.7b07093
38	Qiao B. ; Wang A. ; Yang X. ; Allard L. F. ; Jiang Z. ; Cui Y. ; Liu J. ; Li J. ; Zhang T. Nat. Chem. 2011, 3, 634. doi: 10.1038/nchem.1095
39	Kale M. J. ; Christopher P. ACS Catal. 2016, 6, 5599. doi: 10.1021/acscatal.6b01128
40	Lu Y. ; Wang Y. ; Tang Q. ; Cao Q. ; Fang W. Appl. Catal. B 2022, 300, 120746. doi: 10.1016/j.apcatb.2021.120746
41	Yazawa Y. ; Kagi N. ; Komai S.-I. ; Satsuma A. ; Murakami Y. ; Hattori T. Catal. Lett. 2001, 72, 157. doi: 10.1023/A:1009027926457
42	Zuo F. ; Bozhilov K. ; Dillon R. J. ; Wang L. ; Smith P. ; Zhao X. ; Bardeen C. ; Feng P. Angew. Chem. Int. Ed. 2012, 51, 6223. doi: 10.1002/anie.201202191
43	Qiu C. ; Shen J. ; Lin J. ; Liu D. ; Li D. ; Zhang J. ; Zhang Z. ; Lin H. ; Wang X. ; Fu X. ACS Appl. Energy Mater. 2021, 4, 10172. doi: 10.1021/acsaem.1c02066
44	Caretti I. ; Keulemans M. ; Verbruggen S. W. ; Lenaerts S. ; Van Doorslaer S. Top. Catal. 2015, 58, 776. doi: 10.1007/s11244-015-0419-4
45	Zhang T. ; Lang X. ; Dong A. ; Wan X. ; Gao S. ; Wang L. ; Wang L. ; Wang W. ACS Catal. 2020, 10, 7269. doi: 10.1021/acscatal.0c00703
46	Liu S. ; Huang S. Carbon 2017, 115, 11. doi: 10.1016/j.carbon.2016.12.094

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WO₃-TiO₂负载的Pt单原子催化剂光热协同催化丙烷和丙烯氧化

Photo-Thermo Catalytic Oxidation of C₃H₈ and C₃H₆ over the WO₃-TiO₂ Supported Pt Single-Atom Catalyst

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