Accelerating NADH oxidation and hydrogen production with mid-gap states of nitrogen-rich carbon nitride photocatalyst

Toshali Bhoyar; Dong Jin Kim; B. Moses Abraham; Akanksha Gupta; Nagesh Maile; Nilesh R. Manwar; Surendar Tonda; Devthade Vidyasagar; Suresh S. Umare

doi:10.1016/j.isci.2022.105567

Accelerating NADH oxidation and hydrogen production with mid-gap states of nitrogen-rich carbon nitride photocatalyst

Toshali Bhoyar, Dong Jin Kim, B. Moses Abraham, Akanksha Gupta, Nagesh Maile, Nilesh R. Manwar, Surendar Tonda, Devthade Vidyasagar, Suresh S. Umare

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

15 Scopus citations

Abstract

Regeneration of electron carriers such as NAD⁺/NADH is highly desirable and essential for enzymatic conversions. Here, we demonstrate a sustainable strategy for the regeneration of NAD⁺ as an electron carrier via photon-assisted heterogeneous catalysis. For this, a mid-gap state induced nitrogen-rich polymeric carbon nitride (NPCN) catalyst was synthesized by an additive-assisted thermal copolymerization. Utilizing NPCN as a photocatalyst presented NADH photooxidation efficiency of over 98% and a high hydrogen production rate of 11.18 mmolg⁻¹h⁻¹ with an apparent quantum yield of 9.16% (λ = 420 nm), outperforming other state-of-art metal-free photocatalysts. The experimental and theoretical simulations suggest that mid-gap states in NPCN catalyst are main platform for charge-carrier separation that enhances the overall photocatalytic performance.

Original language	English
Article number	105567
Journal	iScience
Volume	25
Issue number	12
DOIs	https://doi.org/10.1016/j.isci.2022.105567
State	Published - 22 Dec 2022

Bibliographical note

Publisher Copyright:
© 2022 The Authors

Funding

We would like to thank Department of Science and Technology Fund for Improvement of Science and Technology Infrastructure (DST-FIST) through Project No. SR/FST/ CSI-279/2016(C) for providing instrumentation facility at Department of Chemistry, VNIT, Nagpur. We acknowledge SAIF Bombay, SAIF Madras, SAIF NEHU, and IISc Bangalore for their associated support via the central instrumentation facility. TB would like to thank the Director VNIT Nagpur for the doctoral fellowship. BMA acknowledges the HPC center, IIT Kanpur for providing the computational facilities. Conceptualization, T.B. and V.D.; Methodology, T.B. and D.V.; Investigation, T.B. D.J.K. A.G. B.M.A. N.M. N.R.M. S.T. D.V. and S.S.U.; Resources, S.S.U; Formal Analysis, T.B. D.J.K. A.G. B.M.A. N.M. S.T. and D.V.; Visualization, T.B. D.V. and S.S.U.; Writing – Original Draft, T.B.; Writing – Review and Editing, B.M.A. N.R.M. S.T. V.D. and S.S.U.; Supervision, D.V. and S.S.U. Funding Acquisition, S.S.U. The authors declare no competing interests. We support inclusive, diverse, and equitable conduct of research. We would like to thank Department of Science and Technology Fund for Improvement of Science and Technology Infrastructure (DST-FIST) through Project No. SR/FST/ CSI-279/2016(C) for providing instrumentation facility at Department of Chemistry , VNIT , Nagpur. We acknowledge SAIF Bombay , SAIF Madras , SAIF NEHU , and IISc Bangalore for their associated support via the central instrumentation facility. TB would like to thank the Director VNIT Nagpur for the doctoral fellowship. BMA acknowledges the HPC center , IIT Kanpur for providing the computational facilities.

Funders	Funder number
Indian Institute of Science
Department of Science and Technology, Ministry of Science and Technology, India	SR/FST/ CSI-279/2016
Visvesvaraya National Institute of Technology

Keywords

Catalysis
Materials chemistry
Materials science

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.isci.2022.105567

Cite this

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abstract = "Regeneration of electron carriers such as NAD+/NADH is highly desirable and essential for enzymatic conversions. Here, we demonstrate a sustainable strategy for the regeneration of NAD+ as an electron carrier via photon-assisted heterogeneous catalysis. For this, a mid-gap state induced nitrogen-rich polymeric carbon nitride (NPCN) catalyst was synthesized by an additive-assisted thermal copolymerization. Utilizing NPCN as a photocatalyst presented NADH photooxidation efficiency of over 98\% and a high hydrogen production rate of 11.18 mmolg−1h−1 with an apparent quantum yield of 9.16\% (λ = 420 nm), outperforming other state-of-art metal-free photocatalysts. The experimental and theoretical simulations suggest that mid-gap states in NPCN catalyst are main platform for charge-carrier separation that enhances the overall photocatalytic performance.",

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AU - Gupta, Akanksha

AU - Maile, Nagesh

AU - Manwar, Nilesh R.

AU - Tonda, Surendar

AU - Vidyasagar, Devthade

AU - Umare, Suresh S.

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N2 - Regeneration of electron carriers such as NAD+/NADH is highly desirable and essential for enzymatic conversions. Here, we demonstrate a sustainable strategy for the regeneration of NAD+ as an electron carrier via photon-assisted heterogeneous catalysis. For this, a mid-gap state induced nitrogen-rich polymeric carbon nitride (NPCN) catalyst was synthesized by an additive-assisted thermal copolymerization. Utilizing NPCN as a photocatalyst presented NADH photooxidation efficiency of over 98% and a high hydrogen production rate of 11.18 mmolg−1h−1 with an apparent quantum yield of 9.16% (λ = 420 nm), outperforming other state-of-art metal-free photocatalysts. The experimental and theoretical simulations suggest that mid-gap states in NPCN catalyst are main platform for charge-carrier separation that enhances the overall photocatalytic performance.

AB - Regeneration of electron carriers such as NAD+/NADH is highly desirable and essential for enzymatic conversions. Here, we demonstrate a sustainable strategy for the regeneration of NAD+ as an electron carrier via photon-assisted heterogeneous catalysis. For this, a mid-gap state induced nitrogen-rich polymeric carbon nitride (NPCN) catalyst was synthesized by an additive-assisted thermal copolymerization. Utilizing NPCN as a photocatalyst presented NADH photooxidation efficiency of over 98% and a high hydrogen production rate of 11.18 mmolg−1h−1 with an apparent quantum yield of 9.16% (λ = 420 nm), outperforming other state-of-art metal-free photocatalysts. The experimental and theoretical simulations suggest that mid-gap states in NPCN catalyst are main platform for charge-carrier separation that enhances the overall photocatalytic performance.

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Accelerating NADH oxidation and hydrogen production with mid-gap states of nitrogen-rich carbon nitride photocatalyst

Abstract

Bibliographical note

Funding

Keywords

UN SDGs

Access to Document

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