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

iScience. 2022 Nov 12;25(12):105567. doi: 10.1016/j.isci.2022.105567. eCollection 2022 Dec 22.

Authors

Toshali Bhoyar¹, Dong Jin Kim², B Moses Abraham³, Akanksha Gupta⁴, Nagesh Maile⁵, Nilesh R Manwar⁶, Surendar Tonda⁵, Devthade Vidyasagar⁷, Suresh S Umare¹

Affiliations

¹ Materials and Catalysis Laboratory, Visvesvaraya National Institute of Technology (VNIT), Nagpur 440010, India.
² School of Energy Engineering, Kyungpook National University, Buk-gu, Daegu 41566, Republic of Korea.
³ Department of Chemical Engineering, Indian Institute of Technology Kanpur, Kanpur 208016, India.
⁴ Department of Chemistry, Bar-Ilan University, Ramat Gan 5290002, Israel.
⁵ Department of Environmental Engineering, Kyungpook National University, Buk-gu, Daegu 41566, Republic of Korea.
⁶ Department of Chemistry, Institute of Chemical Technology, Matunga, Mumbai 400019, India.
⁷ School of Material Science and Engineering, Kyungpook National University, Daegu 41566, Republic of Korea.

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.

Keywords: Catalysis; Materials chemistry; Materials science.