Hydrogenation of bio-oil-derived oxygenates at ambient conditions via a two-step redox cycle
Hydrogenation of bio-oil-derived oxygenates at ambient conditions via a two-step redox cycle
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DOI：
10.1016/j.xcrp.2023.101506
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发表时间：
2023-07
影响因子：
8.9
通讯作者：
Chongyan Ruan;Ryota Akutsu;Kunran Yang;Noha M. Zayan;Jian Dou;Junchen Liu;A. Bose;Leo Brody;H. Lamb;Fanxing Li
中科院分区：
文献类型：
--
作者：
Chongyan Ruan;Ryota Akutsu;Kunran Yang;Noha M. Zayan;Jian Dou;Junchen Liu;A. Bose;Leo Brody;H. Lamb;Fanxing Li
将生物油升级为可再生燃料和化学品的一个关键挑战在于开发有效且多功能的加氢系统。本文报道了一种两步太阳能热化学加氢工艺，该工艺直接从水和集中的太阳辐射中获取氢气，用于糠醛升级。在室温和大气压下实现了高催化性能，与最先进的催化加氢相比，氢气利用率提高了两个数量级。金属或还原的金属氧化物提供糠醛吸附和水解离的活性位点。原位产生的活性氢原子对糠醛和生物质衍生的含氧化合物进行氢化，消除了氢溶解和随后在催化剂表面解离的障碍。氢化选择性可以通过具有不同极性的溶剂和具有不同亲氧性的金属/还原金属氧化物催化剂来方便地调节。这项工作为生物油升级提供了一种高效且通用的策略，并为可再生能源存储提供了一条有前途的途径。
A key challenge in upgrading bio-oils to renewable fuels and chemicals resides in developing effective and versatile hydrogenation systems. Herein, a two-step solar thermochemical hydrogenation process that sources hydrogen directly from water and concentrated solar radiation for furfural upgrading is reported. High catalytic performance is achieved at room temperature and atmospheric pressure, with up to two-orders-of-magnitude-higher hydrogen utilization efficiency compared with state-of-the-art catalytic hydrogenation. A metal or reduced metal oxide provides the active sites for furfural adsorption and water dissociation. Thein situ-generated reactive hydrogen atoms hydrogenate furfural and biomass-derived oxygenates, eliminating the barriers to hydrogen dissolution and the subsequent dissociation at the catalyst surface. Hydrogenation selectivity can be conveniently mediated by solvents with different polarity and metal/reduced metal oxide catalysts with varying oxophilicity. This work provides an efficient and versatile strategy for bio-oil upgrading and a promising pathway for renewable energy storage.