Volume 62, Issue 38 e202308930

Research Article

Integrated Photochromic-Photothermal Processes for Catalytic Plastic Upcycling

Dr. Yu Liu

Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Soochow University, Suzhou, 215123 P. R. China

These authors contributed equally to this work.

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Dr. Congyang Zhang,

Dr. Congyang Zhang

Department of Chemistry, University of Western Ontario, London, Ontario, N6A 5B7 Canada

These authors contributed equally to this work.

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Dr. Ji Feng,

Dr. Ji Feng

Department of Chemistry, University of California, Riverside, CA, 92521 USA

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Xuchun Wang,

Xuchun Wang

Department of Chemistry, University of Western Ontario, London, Ontario, N6A 5B7 Canada

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Prof. Dr. Zhifeng Ding,

Prof. Dr. Zhifeng Ding

Department of Chemistry, University of Western Ontario, London, Ontario, N6A 5B7 Canada

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Prof. Dr. Le He,

Prof. Dr. Le He

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Prof. Dr. Qiao Zhang,

Prof. Dr. Qiao Zhang

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Prof. Dr. Jinxing Chen,

Corresponding Author

Prof. Dr. Jinxing Chen

[email protected]

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Prof. Dr. Yadong Yin,

Corresponding Author

Prof. Dr. Yadong Yin

[email protected]

orcid.org/0000-0003-0218-3042

Department of Chemistry, University of California, Riverside, CA, 92521 USA

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Dr. Yu Liu,

Dr. Yu Liu

These authors contributed equally to this work.

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Dr. Congyang Zhang,

Dr. Congyang Zhang

Department of Chemistry, University of Western Ontario, London, Ontario, N6A 5B7 Canada

These authors contributed equally to this work.

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Dr. Ji Feng,

Dr. Ji Feng

Department of Chemistry, University of California, Riverside, CA, 92521 USA

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Xuchun Wang,

Xuchun Wang

Department of Chemistry, University of Western Ontario, London, Ontario, N6A 5B7 Canada

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Prof. Dr. Zhifeng Ding,

Prof. Dr. Zhifeng Ding

Department of Chemistry, University of Western Ontario, London, Ontario, N6A 5B7 Canada

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Prof. Dr. Le He,

Prof. Dr. Le He

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Prof. Dr. Qiao Zhang,

Prof. Dr. Qiao Zhang

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Prof. Dr. Jinxing Chen,

Corresponding Author

Prof. Dr. Jinxing Chen

[email protected]

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Prof. Dr. Yadong Yin,

Corresponding Author

Prof. Dr. Yadong Yin

[email protected]

orcid.org/0000-0003-0218-3042

Department of Chemistry, University of California, Riverside, CA, 92521 USA

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First published: 01 August 2023

https://doi.org/10.1002/anie.202308930

Citations: 12

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Graphical Abstract

We surpass the limitation of the existing photothermal catalysis mechanism and propose a photochromic-photothermal catalytic system based on polyol-ligated TiO₂ nanocrystals. Upon sunlight irradiation, the chemically bonded polyols capture holes generated by TiO₂, enabling photogenerated electrons to reduce Ti⁴⁺ to Ti³⁺ and produce oxygen vacancies. This process boosts photothermal efficiency and facilitates polyester glycolysis efficiency.

Abstract

Incorporating high-energy ultraviolet (UV) photons into photothermal catalytic processes may enable photothermal-photochemical synergistic catalysis, which represents a transformative technology for waste plastic recycling. The major challenge is avoiding side reactions and by-products caused by these energetic photons. Here, we break through the limitation of the existing photothermal conversion mechanism and propose a photochromic-photothermal catalytic system based on polyol-ligated TiO₂ nanocrystals. Upon UV or sunlight irradiation, the chemically bonded polyols can rapidly capture holes generated by TiO₂, enabling photogenerated electrons to reduce Ti⁴⁺ to Ti³⁺ and produce oxygen vacancies. The resulting abundant defect energy levels boost sunlight-to-heat conversion efficiency, and simultaneously the oxygen vacancies facilitate polyester glycolysis by activating the nucleophilic addition-elimination process. As a result, compared to commercial TiO₂ (P25), we achieve 6-fold and 12.2-fold performance enhancements under thermal and photothermal conditions, respectively, while maintaining high selectivity to high-valued monomers. This paradigm-shift strategy directs energetic UV photons for activating catalysts and avoids their interaction with reactants, opening the possibility of substantially elevating the efficiency of more solar-driven catalysis.

Conflict of interest

The authors declare no conflict of interest.

Open Research

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

Supporting Information

References

1
1aC. Zhang, Q. Kang, M. Chu, L. He, J. Chen, Trends Chem. 2022, 4, 822–834;
10.1016/j.trechm.2022.06.005
CAS Web of Science® Google Scholar
1bX. Jiao, K. Zheng, Z. Hu, S. Zhu, Y. Sun, Y. Xie, Adv. Mater. 2021, 33, 2005192.
10.1002/adma.202005192
CAS PubMed Web of Science® Google Scholar
2
2aS. Chu, B. Zhang, X. Zhao, H. S. Soo, F. Wang, R. Xiao, H. Zhang, Adv. Energy Mater. 2022, 12, 2200435;
10.1002/aenm.202200435
CAS Web of Science® Google Scholar
2bU. Taylor, K. Hatice, R. Erwin, J. Am. Chem. Soc. 2019, 141, 15201–15210;
10.1021/jacs.8b13633
PubMed Web of Science® Google Scholar
2cR. Cao, M. Zhang, C. Hu, D. Xiao, M. Wang, D. Ma, Nat. Commun. 2022, 13, 4809.
10.1038/s41467-022-32510-x
CAS PubMed Web of Science® Google Scholar
3
3aJ. Ye, Y. Chen, C. Gao, C. Wang, A. Hu, G. Dong, Z. Chen, S. Zhou, Y. Xiong, Angew. Chem. Int. Ed. 2022, 61, e202213244;
10.1002/anie.202213244
CAS PubMed Web of Science® Google Scholar
3bX. Jiao, K. Zheng, Q. Chen, X. Li, Y. Li, W. Shao, J. Xu, J. Zhu, Y. Pan, Y. Sun, Y. Xie, Angew. Chem. Int. Ed. 2020, 59, 15497–15501.
10.1002/anie.201915766
CAS PubMed Web of Science® Google Scholar
4
4aM. Zhang, M. Wang, S. Bo, C. Hu, D. Xiao, D. Ma, Chem 2022, 8, 2912–2923;
10.1016/j.chempr.2022.08.004
CAS Web of Science® Google Scholar
4bY. Liu, Q. Zhong, P. Xu, H. Huang, F. Yang, M. Cao, L. He, Q. Zhang, J. Chen, Matter 2022, 5, 1305–1317;
10.1016/j.matt.2022.02.002
CAS Web of Science® Google Scholar
4cPlastic upcycling. Nat. Catal. 2019, 2, 945–946.
Google Scholar
5
5aF. Yu, C. Wang, Y. Li, H. Ma, R. Wang, Y. Liu, N. Suzuki, C. Terashima, B. Ohtani, T. Ochiai, A. Fujishima, X. Zhang, Adv. Sci. 2020, 7, 2000204;
10.1002/advs.202000204
CAS Web of Science® Google Scholar
5bM. Cai, Z. Wu, Z. Li, L. Wang, W. Sun, A. A. Tountas, C. Li, S. Wang, K. Feng, A.-B. Xu, S. Tang, A. Tavasoli, M. Peng, W. Liu, A. S. Helmy, L. He, G. A. Ozin, X. Zhang, Nat. Energy 2021, 6, 807–814.
10.1038/s41560-021-00867-w
CAS Web of Science® Google Scholar
6
6aC. Song, Z. Wang, Z. Yin, D. Xiao, D. Ma, Chem Catal. 2022, 2, 52–83;
10.1016/j.checat.2021.10.005
CAS Web of Science® Google Scholar
6bY. Zhao, W. Gao, S. Li, G. R. Williams, A. H. Mahadi, D. Ma, Joule 2019, 3, 920–937.
10.1016/j.joule.2019.03.003
CAS Web of Science® Google Scholar
7
7aP. Xu, Q. Dai, H. Gao, H. Liu, M. Zhang, M. Li, Y. Chen, K. An, Y. S. Meng, P. Liu, Y. Li, J. S. Spangenberger, L. Gaines, J. Lu, Z. Chen, Joule 2020, 4, 2609–2626;
10.1016/j.joule.2020.10.008
CAS Web of Science® Google Scholar
7bK. Kimoto, T. Asaka, T. Nagai, M. Saito, Y. Matsui, K. Ishizuka, Nature 2007, 450, 702–704.
10.1038/nature06352
CAS PubMed Web of Science® Google Scholar
8Y. Guo, S. Chen, Y. Yu, H. Tian, Y. Zhao, J. C. Ren, C. Huang, H. Bian, M. Huang, L. An, Y. Li, R. Zhang, J. Am. Chem. Soc. 2019, 141, 8407–8411.
10.1021/jacs.9b01836
CAS PubMed Web of Science® Google Scholar
9Q. Zhong, J. Feng, B. Jiang, Y. Fan, Q. Zhang, J. Chen, Y. Yin, J. Am. Chem. Soc. 2021, 143, 20513–20523.
10.1021/jacs.1c11242
CAS PubMed Web of Science® Google Scholar
10X. Cao, Z. Chen, R. Lin, W. Cheong, S. Liu, J. Zhang, Q. Peng, C. Chen, T. Han, X. Tong, Y. Wang, R. Shen, W. Zhu, D. Wang, Y. Li, Nat. Catal. 2018, 1, 704–710.
10.1038/s41929-018-0128-z
CAS Web of Science® Google Scholar
11A. Naldoni, M. Altomare, G. Zoppellaro, N. Liu, S. Kment, R. Zboril, P. Schmuki, ACS Catal. 2019, 9, 345–364.
10.1021/acscatal.8b04068
CAS PubMed Web of Science® Google Scholar
12X. Chen, L. Liu, P. Y. Yu, S. S. Mao, Science 2011, 331, 746–750.
10.1126/science.1200448
CAS PubMed Web of Science® Google Scholar
13
13aM. Ghoussoub, M. Xia, P. N. Duchesne, D. Segal, G. Ozin, Energy Environ. Sci. 2019, 12, 1122–1142;
10.1039/C8EE02790K
CAS Web of Science® Google Scholar
13bH. Lin, S. Luo, H. Zhang, Y. Jinhua, Joule 2022, 6, 294–314;
10.1016/j.joule.2022.01.001
CAS Web of Science® Google Scholar
13cH. Huang, R. Shi, X. Zhang, J. Zhao, C. Su, T. Zhang, Angew. Chem. Int. Ed. 2021, 60, 22963–22969.
10.1002/anie.202110336
CAS PubMed Web of Science® Google Scholar
14S. Wang, D. Zhang, W. Wang, J. Zhong, K. Feng, Z. Wu, B. Du, J. He, Z. Li, L. He, W. Sun, D. Yang, G. A. Ozin, Nat. Commun. 2022, 13, 5303.
10.1038/s41467-022-33027-z
PubMed Web of Science® Google Scholar
15R. Aleisa, J. Feng, Z. Ye, Y. Yin, Angew. Chem. Int. Ed. 2022, 61, e202203700.
10.1002/anie.202203700
CAS PubMed Web of Science® Google Scholar
16Z. Zhang, Q. Wu, G. Johnson, Y. Ye, X. Li, N. Li, M. Cui, J. D. Lee, C. Liu, S. Zhao, S. Li, A. Orlov, C. B. Murray, X. Zhang, T. B. Gunnoe, D. Su, S. Zhang, J. Am. Chem. Soc. 2019, 141, 16548–16552.
10.1021/jacs.9b06389
CAS PubMed Web of Science® Google Scholar
17A. Naldoni, M. Allieta, S. Santangelo, M. Marelli, F. Fabbri, S. Cappelli, C. L. Bianchi, R. Psaro, V. Dal Santo, J. Am. Chem. Soc. 2012, 134, 7600–7603.
10.1021/ja3012676
CAS PubMed Web of Science® Google Scholar
18W. Zhou, W. Li, J. Wang, Y. Qu, Y. Yang, Y. Xie, K. Zhang, L. Wang, H. Fu, D. Zhao, J. Am. Chem. Soc. 2014, 136, 9280–9283.
10.1021/ja504802q
CAS PubMed Web of Science® Google Scholar
19
19aR. Ma, K. Fukuda, T. Sasaki, M. Osada, Y. Bando, J. Phys. Chem. B 2005, 109, 6210–6214;
10.1021/jp044282r
CAS PubMed Web of Science® Google Scholar
19bC. Foo, Y. Li, K. Lebedev, T. Chen, S. Day, C. Tang, S. C. E. Tsang, Nat. Commun. 2021, 12, 661.
10.1038/s41467-021-20977-z
CAS PubMed Web of Science® Google Scholar
20N. O. Gopal, H.-H. Lo, S.-C. Sheu, S.-C. Ke, J. Am. Chem. Soc. 2010, 132, 10982–10983.
10.1021/ja909901f
CAS PubMed Web of Science® Google Scholar
21
21aG. Kresse, J. Furthmuller, Phys. Rev. B 1996, 54, 16;
10.1103/PhysRevB.54.11169
Web of Science® Google Scholar
21bJ. P. Perdew, J. A. Chevary, S. H. Vosko, K. A. Jackson, M. R. Pederson, D. J. Singh, C. Fiolhais, Phys. Rev. B 1992, 46, 6671–6687;
10.1103/PhysRevB.46.6671
CAS PubMed Web of Science® Google Scholar
21cP. E. Blöchl, Phys. Rev. B 1994, 50, 17953–17979.
10.1103/PhysRevB.50.17953
CAS PubMed Web of Science® Google Scholar
22C. Jehanno, J. Demarteau, D. Mantione, M. C. Arno, F. Ruiperez, J. L. Hedrick, A. P. Dove, H. Sardon, Angew. Chem. Int. Ed. 2021, 60, 6710–6717.
10.1002/anie.202014860
CAS PubMed Web of Science® Google Scholar
23M. L. Knotek, Rep. Prog. Phys. 1984, 47, 1499.
10.1088/0034-4885/47/11/002
CAS Web of Science® Google Scholar
24L. Gao, X. Cui, Z. Wang, C. D. Sewell, Z. Li, S. Liang, Z. Lin, Proc. Natl. Acad. Sci. USA 2021, 118, e2023421118.
10.1073/pnas.2023421118
CAS PubMed Web of Science® Google Scholar
25M. Zhang, W. Chen, W. Choi, J. Yu, Y. Deng, X. Xie, Z. Lin, ACS Sustainable Chem. Eng. 2022, 10, 4741–4749.
10.1021/acssuschemeng.2c00416
CAS Web of Science® Google Scholar

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Volume62, Issue38

September 18, 2023

e202308930

Integrated Photochromic-Photothermal Processes for Catalytic Plastic Upcycling

Graphical Abstract

Abstract

Conflict of interest

Open Research

Data Availability Statement

Supporting Information

References

Citing Literature

References

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Integrated Photochromic-Photothermal Processes for Catalytic Plastic Upcycling

Graphical Abstract

Abstract

Conflict of interest

Open Research

Data Availability Statement

Supporting Information

References

Citing Literature

References

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