Understanding Photocatalytic Activity Dependence on Node Topology in Ti-Based Metal–Organic Frameworks

Nikita Kolobov; Abdelali Zaki; Katarzyna Świrk; Partha Maity; Luis Carlos Garzon Tovar; Giasemi K. Angeli; Alla Dikhtiarenko; G. Delahay; Pantelis N. Trikalitis; Abdul-Hamid M. Emwas; Amandine Cadiau; Omar F. Mohammed; Christopher H. Hendon; Karim Adil; Jorge Gascon

doi:10.1021/acsmaterialslett.2c01115

Understanding Photocatalytic Activity Dependence on Node Topology in Ti-Based Metal–Organic Frameworks

Nikita Kolobov, Abdelali Zaki, Katarzyna Świrk, Partha Maity, Luis Carlos Garzon Tovar, Giasemi K. Angeli, Alla Dikhtiarenko, G. Delahay, Pantelis N. Trikalitis, Abdul-Hamid M. Emwas, Amandine Cadiau, Omar F. Mohammed, Christopher H. Hendon, Karim Adil, Jorge Gascon

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6 Scopus citations

Abstract

Despite the drive to develop more efficient Ti-based metal–organic framework (MOF) photocatalysts, MIL-125-NH2 is still the benchmark, and only a few design principles have been offered to improve photocatalytic performance. Linker functionalization in Ti MOFs has been shown to enable photocatalysis under visible light by closing the electronic band gap, significantly improving charge carrier lifetimes. Limited by known Ti-based MOFs, the role of node nuclearity and topology on photocatalytic activity remains unclear. Here, we report a new MOF, ICGM-1, a 3D-connected framework featuring 1D Ti–O rods. Photocatalytic hydrogen evolution reveals a significant difference in activity, which we attribute solely to node geometry. Using time-resolved spectroscopy and DFT calculations, we ascribe these differences to subtle electronic and geometric properties, paving the way for the development of Ti-MOF photocatalysts.

Original language	English (US)
Pages (from-to)	1481-1487
Number of pages	7
Journal	ACS Materials Letters
DOIs	https://doi.org/10.1021/acsmaterialslett.2c01115
State	Published - Apr 17 2023

Bibliographical note

KAUST Repository Item: Exported on 2023-05-05
Acknowledgements: Funding for this work was provided by King Abdullah University of Science and Technology (KAUST). Funding for this work was provided by King Abdullah University of Science and Technology (KAUST) This work is based upon work supported by the National Science Foundation through the Division of Materials Research under Grant No. DMR-1956403. C.H.H. also acknowledges the Camille and Henry Dreyfus Foundation.

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10.1021/acsmaterialslett.2c01115

https://repository.kaust.edu.sa/bitstream/10754/691451/1/acsmaterialslett.2c01115.pdf

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Kolobov, N., Zaki, A., Świrk, K., Maity, P., Garzon Tovar, L. C., Angeli, G. K., Dikhtiarenko, A., Delahay, G., Trikalitis, P. N., Emwas, A.-H. M., Cadiau, A., Mohammed, O. F., Hendon, C. H., Adil, K., & Gascon, J. (2023). Understanding Photocatalytic Activity Dependence on Node Topology in Ti-Based Metal–Organic Frameworks. ACS Materials Letters, 1481-1487. https://doi.org/10.1021/acsmaterialslett.2c01115

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title = "Understanding Photocatalytic Activity Dependence on Node Topology in Ti-Based Metal–Organic Frameworks",

abstract = "Despite the drive to develop more efficient Ti-based metal–organic framework (MOF) photocatalysts, MIL-125-NH2 is still the benchmark, and only a few design principles have been offered to improve photocatalytic performance. Linker functionalization in Ti MOFs has been shown to enable photocatalysis under visible light by closing the electronic band gap, significantly improving charge carrier lifetimes. Limited by known Ti-based MOFs, the role of node nuclearity and topology on photocatalytic activity remains unclear. Here, we report a new MOF, ICGM-1, a 3D-connected framework featuring 1D Ti–O rods. Photocatalytic hydrogen evolution reveals a significant difference in activity, which we attribute solely to node geometry. Using time-resolved spectroscopy and DFT calculations, we ascribe these differences to subtle electronic and geometric properties, paving the way for the development of Ti-MOF photocatalysts.",

author = "Nikita Kolobov and Abdelali Zaki and Katarzyna {\'S}wirk and Partha Maity and {Garzon Tovar}, {Luis Carlos} and Angeli, {Giasemi K.} and Alla Dikhtiarenko and G. Delahay and Trikalitis, {Pantelis N.} and Emwas, {Abdul-Hamid M.} and Amandine Cadiau and Mohammed, {Omar F.} and Hendon, {Christopher H.} and Karim Adil and Jorge Gascon",

note = "KAUST Repository Item: Exported on 2023-05-05 Acknowledgements: Funding for this work was provided by King Abdullah University of Science and Technology (KAUST). Funding for this work was provided by King Abdullah University of Science and Technology (KAUST) This work is based upon work supported by the National Science Foundation through the Division of Materials Research under Grant No. DMR-1956403. C.H.H. also acknowledges the Camille and Henry Dreyfus Foundation.",

year = "2023",

month = apr,

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doi = "10.1021/acsmaterialslett.2c01115",

language = "English (US)",

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journal = "ACS Materials Letters",

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Kolobov, N, Zaki, A, Świrk, K, Maity, P , Garzon Tovar, LC, Angeli, GK, Dikhtiarenko, A, Delahay, G, Trikalitis, PN, Emwas, A-HM, Cadiau, A, Mohammed, OF, Hendon, CH, Adil, K & Gascon, J 2023, 'Understanding Photocatalytic Activity Dependence on Node Topology in Ti-Based Metal–Organic Frameworks', ACS Materials Letters, pp. 1481-1487. https://doi.org/10.1021/acsmaterialslett.2c01115

TY - JOUR

T1 - Understanding Photocatalytic Activity Dependence on Node Topology in Ti-Based Metal–Organic Frameworks

AU - Kolobov, Nikita

AU - Zaki, Abdelali

AU - Świrk, Katarzyna

AU - Maity, Partha

AU - Garzon Tovar, Luis Carlos

AU - Angeli, Giasemi K.

AU - Dikhtiarenko, Alla

AU - Delahay, G.

AU - Trikalitis, Pantelis N.

AU - Emwas, Abdul-Hamid M.

AU - Cadiau, Amandine

AU - Mohammed, Omar F.

AU - Hendon, Christopher H.

AU - Adil, Karim

AU - Gascon, Jorge

N1 - KAUST Repository Item: Exported on 2023-05-05 Acknowledgements: Funding for this work was provided by King Abdullah University of Science and Technology (KAUST). Funding for this work was provided by King Abdullah University of Science and Technology (KAUST) This work is based upon work supported by the National Science Foundation through the Division of Materials Research under Grant No. DMR-1956403. C.H.H. also acknowledges the Camille and Henry Dreyfus Foundation.

PY - 2023/4/17

Y1 - 2023/4/17

N2 - Despite the drive to develop more efficient Ti-based metal–organic framework (MOF) photocatalysts, MIL-125-NH2 is still the benchmark, and only a few design principles have been offered to improve photocatalytic performance. Linker functionalization in Ti MOFs has been shown to enable photocatalysis under visible light by closing the electronic band gap, significantly improving charge carrier lifetimes. Limited by known Ti-based MOFs, the role of node nuclearity and topology on photocatalytic activity remains unclear. Here, we report a new MOF, ICGM-1, a 3D-connected framework featuring 1D Ti–O rods. Photocatalytic hydrogen evolution reveals a significant difference in activity, which we attribute solely to node geometry. Using time-resolved spectroscopy and DFT calculations, we ascribe these differences to subtle electronic and geometric properties, paving the way for the development of Ti-MOF photocatalysts.

AB - Despite the drive to develop more efficient Ti-based metal–organic framework (MOF) photocatalysts, MIL-125-NH2 is still the benchmark, and only a few design principles have been offered to improve photocatalytic performance. Linker functionalization in Ti MOFs has been shown to enable photocatalysis under visible light by closing the electronic band gap, significantly improving charge carrier lifetimes. Limited by known Ti-based MOFs, the role of node nuclearity and topology on photocatalytic activity remains unclear. Here, we report a new MOF, ICGM-1, a 3D-connected framework featuring 1D Ti–O rods. Photocatalytic hydrogen evolution reveals a significant difference in activity, which we attribute solely to node geometry. Using time-resolved spectroscopy and DFT calculations, we ascribe these differences to subtle electronic and geometric properties, paving the way for the development of Ti-MOF photocatalysts.

UR - http://hdl.handle.net/10754/691451

UR - https://pubs.acs.org/doi/10.1021/acsmaterialslett.2c01115

U2 - 10.1021/acsmaterialslett.2c01115

DO - 10.1021/acsmaterialslett.2c01115

M3 - Article

SN - 2639-4979

SP - 1481

EP - 1487

JO - ACS Materials Letters

JF - ACS Materials Letters

ER -

Understanding Photocatalytic Activity Dependence on Node Topology in Ti-Based Metal–Organic Frameworks

Abstract

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