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Melem (M) is an emergent metal‐free material due to its nature abundance and easy preparation. Synergetic escalation of band gap generation and charge transfer of M to increase solar chemical synthesis ability remains a hot challenging topic yet. Herein, we designed first time in‐situ prepared sulfur‐doped covalent melem‐based frameworks (S‐CMFs) photocatalyst for NAD(P)H regeneration and 1,3‐oxathiolane‐2‐thiones production under solar light irradiation. S‐CMFs photocatalyst shows excellent photocatalytic stability and activity over the pristine CMFs and M. The presence of sulfur in frameworks drastically improved the photocatalytic efficiency of S‐CMFs due to its unique properties such as enhanced the solar light adsorption ability, molar extinction coefficient, slow charge recombination, fast charge separation and transportation of solar light to generate electrons‐holes. Hence, S‐CMFs photocatalyst has a vital role in the regeneration of NADH and NADPH with 54.84 and 51.05 % catalytic efficiencies and ~ 99 % for yields and selectivity of 1,3‐oxathiolane‐2‐thiones under solar light. This study demonstrates that the Z‐scheme hetero junction and photocatalytic reaction using S‐CMFs would be a suitable route for the production of solar fuel via artificial photosynthetic system.

Covalent organic frameworks (COFs) exhibit excellent characteristics in the optoelectronic and photocatalytic areas. The broad demand for highly efficient flexible clothes enhances the investigation of multifarious COFs materials. Currently, COFs have materialized as future generation flexible clothes layered materials with previously designed π‐π stacking skeletons and extremely efficient ordered structures, which are more fascinated for countering their photocatalytic characteristics. Still, COFs are generally formed as solid materials because of direction‐dependent growth which make them unpredictable to integrate into flexible clothes. Here, by choosing tetraamino‐benzoquinone (T) and N,N'‐di‐(4‐benzoic acid)‐perylene‐3,4,9,10‐tetracarboxylic acid diimide (BP) monomers with photocatalytic activity, ornately designed sun‐light‐responsive COFs with well‐ordered donor and acceptor moieties are in situsynthesized on flexible activated carbon cloth (fACC), eventually forming TBPCOF‐fACC structures. Ultra‐responsive photocatalyst is fruitfully fabricated with the TBPCOF‐fACC structure and showed an excellent selective C‐S arylation performance with high yields (99 %) at ambient temperature. The research presents new plans for constructions of advanced light harvesting functional flexible clothes with programmable COFs material, covering the technique for a creation of highly improved applications in photocatalytic and various areas. The TBPCOF‐fACC based humidity sensor shows the average sensitivity as 1.58 MΩ/%RH along with calculated response and recovery time as 15 s and 55 s respectively. The sensor has 96.20 % repeatability and shows long term stability.

In artificial photosynthesis process the photocatalyst‐enzyme attached system is a best strategy to utilize solar energy for solar chemical/fuels production. Herein, we prepared a solar light active graphene‐based photocatalyst received by the covalent attachment of 9‐aminoanthracene (AA) chromophore with chemically converted graphene (CCG) for highly efficient 1,4‐NADH regeneration (79.9 %) and conversion of α‐ketoglutarate (α‐KG) in to L‐glutamate (L‐GM) (88.3 %) in 2 hrs. The present result is a benchmark example of highly selective solar light active enzyme based artificial photosynthetic system for selective formation of L‐GM from α‐KG.