Lu Yuan, Liu Tae-Kyung, Lin Cheng, Kim Kwang Hee, Kim Eugene, Yang Yan, Fan Xinyi, Zhang Kan, Park Jong Hyeok
Department of Chemical and Biomolecular Engineering, Yonsei-KIST Convergence Research Institute, Yonsei University, 50 Yonsei-ro, Seodaemun-gu, Seoul 120-749, Republic of Korea.
School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
Nano Lett. 2024 Apr 17;24(15):4633-4640. doi: 10.1021/acs.nanolett.4c00791. Epub 2024 Apr 3.
The glycerol oxidation reaction (GOR) run with photoelectrochemical cells (PECs) is one of the most promising ways to upgrade biomass because it is thermodynamically favorable, while irreversible overoxidation leads to unsatisfactory product selectivities. Herein, a tunable one-dimensional nanoconfined environment was introduced into the GOR process, which accelerated mass transfer of glycerol via the microscale fluid effect and changed the main oxidation product from formic acid (FA) to glyceraldehyde (GLD), which led to retention of the heavier multicarbon products. The rate of glycerol diffusion in the nanochannels increased by a factor of 4.92 with decreasing inner diameters. The main product from the PEC-selective oxidation of glycerol changed from the C1 product FA to the C3 product GLD with a great selectivity of 60.7%. This work provides a favorable approach for inhibiting further oxidation of multicarbon products and illustrates the importance of microenvironmental regulation in biomass oxidation.
利用光电化学电池（PEC）进行甘油氧化反应（GOR）是生物质升级最具前景的方法之一，因为该反应在热力学上是有利的，然而不可逆的过度氧化会导致产物选择性不尽人意。在此，将一种可调节的一维纳米受限环境引入到GOR过程中，该环境通过微尺度流体效应加速了甘油的传质，并将主要氧化产物从甲酸（FA）转变为甘油醛（GLD），从而使得较重的多碳产物得以保留。随着内径减小，甘油在纳米通道中的扩散速率提高了4.92倍。PEC对甘油的选择性氧化的主要产物从C1产物FA转变为C3产物GLD，选择性高达60.7%。这项工作为抑制多碳产物的进一步氧化提供了一种有利的方法，并阐明了微环境调控在生物质氧化中的重要性。
