Investigation of Water‐Stable Perovskite DMASnI_xBr_3−x for Photoenzyme Catalysis in Aqueous Solution

Abstract

The impressive optoelectronic performances of hybrid perovskites have attracted enormous interests. However, the moisture sensitivity of these materials hampers their practical applications. Herein, the lead‐free perovskites of DMASnIxBr3−x (DMA = CH3NH2CH3+) crystals as photocatalysts for nicotinamide adenine dinucleotide (NADH) regeneration in aqueous solution are engineered. The very high NADH yield (≈100%) is achieved for all the DMASnIxBr3−x crystals with tunable bandgaps, which is further coupled with formate dehydrogenase for the production of 320 μM formic acid from CO2. The density functional theory (DFT) calculations further shed light on the intrinsic water‐stable mechanism of DMASnI3 perovskite, which is ascribed to the higher water surface adsorption energy, the higher water osmotic energy barrier, and the smaller intralayer spacing inside DMASnI3 structures by comparing with Pb‐based counterpart. The work can provide new prospects for designing water‐stable hybrid perovskites and further broaden their photocatalytic and optoelectronic applications.

Water-stable and hydrophobicity tunable organolead halide materials with Pb–N coordination for electrochemical CO2 reduction

“…However, both are much higher than those of superstar hybrid perovskites, such as MAPbI 3 , MASnI 3 and MAGeI 3 (Fig. 3f and Table S2 †), 32,[38][39][40][41] conrming the much stronger osmotic barrier effect of APbX 2 exposed to moisture. The thermal stability of APbX 2 materials was also investigated by the thermogravimetric analysis.…”

“…3c and S9 †). [30][31][32] The hydrophobicity can effectively prevent the penetration of moisture and strengthen the water stability. [33][34][35][36][37] To conrm this, inltration processes of the water molecule into 4,4BpyPbCl 2 and 4,4BpyPbI 2 were explored, as shown in Fig.…”

Lead-free hybrid perovskite photocatalysts: surface engineering, charge-carrier behaviors, and solar-driven applications

“…In addition, DMASnI x Br 3− x exhibits excellent performance for NADH production, reaching 100%, in addition to a formic acid yield of 320 μM from CO 2 . 211…”

Bioinspired Metalation of the Metal‐Organic Framework MIL‐125‐NH2 for Photocatalytic NADH Regeneration and Gas‐Liquid‐Solid Three‐Phase Enzymatic CO2 Reduction

“…[16][17][18] Photocatalytic NADH regeneration usually occurs in the presence of photocatalysts as well as homogeneous metal complex (such as [Cp*Rh(bpy)H 2 O] 2 + ), which act as the electron and proton mediator. [19][20][21][22][23][24][25] Previously, most of the photoinduced electrons were transferred from the heterogeneous semiconductor particles to the homogeneous Rh complex to accomplish the first step of the photocatalytic NADH regeneration, which could pose severe electron transfer loss. Moreover, the homogeneous Rh complex is prone to poisoning enzymes, reducing the reaction efficiency.…”