TY - JOUR

T1 - Coordination between electron transfer and molecule diffusion through a bioinspired amorphous titania nanoshell for photocatalytic nicotinamide cofactor regeneration

AU - Yang, Dong

AU - Zhang, Yishan

AU - Zhang, Shaohua

AU - Cheng, Yuqing

AU - Wu, Yizhou

AU - Cai, Ziyi

AU - Wang, Xiaodong

AU - Shi, Jiafu

AU - Jiang, Zhongyi

N1 - This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acscatal.9b03462

PY - 2019/12/6

Y1 - 2019/12/6

N2 - In-depth understanding and rational manipulation of the electron transfer process and molecule diffusion process are critical to promote the overall photocatalytic efficiency. In our study, core@shell photocatalysts that embody graphitic carbon nitride (GCN) core and amorphous titania (a-TiO 2) nanoshell are prepared to elucidate and coordinate the electron transfer and molecule diffusion for the regeneration of nicotinamide adenine dinucleotide (NADH) with [Cp*Rh(bpy)H 2O] 2+ as the redox mediator. The GCN core absorbs visible light to generate electron-hole pairs, whereas the a-TiO 2 nanoshell facilitates the transfer of photogenerated electrons from GCN to the a-TiO 2 surface for NADH regeneration, which also enables the diffusion of electron donor molecules (triethanolamine, TEOA) from the a-TiO 2 surface to GCN for consuming the holes left on GCN. The transfer of photogenerated electrons and the diffusion of electron donor molecules are coordinated by finely tuning the thickness of the a-TiO 2 nanoshell. Under the optimized nanoshell thickness of â¼2.1 nm, the GCN@a-TiO 2 photocatalyst exhibits the highest NADH regeneration yield of 82.1% after a 10 min reaction under LED light (405 nm), over 200% higher than that of the GCN photocatalyst. Combined with the highly controllable and mild features of the bioinspired mineralization method, our study may offer a facile and generic strategy to design high performance photocatalysts through rational coordination of different substances/species transport processes.

AB - In-depth understanding and rational manipulation of the electron transfer process and molecule diffusion process are critical to promote the overall photocatalytic efficiency. In our study, core@shell photocatalysts that embody graphitic carbon nitride (GCN) core and amorphous titania (a-TiO 2) nanoshell are prepared to elucidate and coordinate the electron transfer and molecule diffusion for the regeneration of nicotinamide adenine dinucleotide (NADH) with [Cp*Rh(bpy)H 2O] 2+ as the redox mediator. The GCN core absorbs visible light to generate electron-hole pairs, whereas the a-TiO 2 nanoshell facilitates the transfer of photogenerated electrons from GCN to the a-TiO 2 surface for NADH regeneration, which also enables the diffusion of electron donor molecules (triethanolamine, TEOA) from the a-TiO 2 surface to GCN for consuming the holes left on GCN. The transfer of photogenerated electrons and the diffusion of electron donor molecules are coordinated by finely tuning the thickness of the a-TiO 2 nanoshell. Under the optimized nanoshell thickness of â¼2.1 nm, the GCN@a-TiO 2 photocatalyst exhibits the highest NADH regeneration yield of 82.1% after a 10 min reaction under LED light (405 nm), over 200% higher than that of the GCN photocatalyst. Combined with the highly controllable and mild features of the bioinspired mineralization method, our study may offer a facile and generic strategy to design high performance photocatalysts through rational coordination of different substances/species transport processes.

U2 - 10.1021/acscatal.9b03462

DO - 10.1021/acscatal.9b03462

M3 - Journal article

VL - 9

SP - 11492

EP - 11501

JO - ACS Catalysis

JF - ACS Catalysis

SN - 2155-5435

IS - 12

ER -