Li Xianghong, Zhang Peng, Yang Chengsheng, Wang Zhongyan, Song Xiwen, Wang Tuo, Gong Jinlong
School of Chemical Engineering & Technology, Key Laboratory for Green Chemical Technology of Ministry of Education, Tianjin University, Tianjin, 300072, China.
Collaborative Innovation Center of Chemical Science & Engineering (Tianjin), Tianjin, 300072, China.
Angew Chem Int Ed Engl. 2023 Aug 21;62(34):e202301901. doi: 10.1002/anie.202301901. Epub 2023 Jul 17.
Construction of a "net-zero-emission" system through CO hydrogenation to methanol with solar energy is an eco-friendly way to mitigate the greenhouse effect. Traditional CO hydrogenation demands centralized mass production for cost reduction with mass water electrolysis for hydrogen supply. To achieve continuous reaction with intermittent and fluctuating flow of H on a small-scale for distributed application scenarios, modulating the catalyst interface environment and chemical adsorption capacity to adapt fluctuating reaction conditions is highly desired. This paper describes a distributed clean CO utilization system in which the surface structure of catalysts is carefully regulated. The Ni catalyst with unsaturated electrons loaded on In O can reduce the dissociation energy of H to overcome the slow response of intermittent H supply, exhibiting a faster response (12 min) than bare oxide catalysts (42 min). Moreover, the introduction of Ni enhances the sensitivity of the catalyst to hydrogen, yielding a Ni/In O catalyst with a good performance at lower H concentrations with a 15 times adaptability for wider hydrogen fluctuation range than In O , greatly reducing the negative impact of unstable H supplies derived from renewable energies.
通过太阳能将一氧化碳加氢制甲醇构建“净零排放”系统是减轻温室效应的一种环保方式。传统的一氧化碳加氢需要集中大规模生产以降低成本,并通过大规模水电解来供应氢气。为了在小规模分布式应用场景中实现与间歇性和波动的氢气流量的连续反应,非常需要调节催化剂界面环境和化学吸附能力以适应波动的反应条件。本文描述了一种分布式清洁一氧化碳利用系统,其中催化剂的表面结构得到了精心调控。负载在氧化铟上的具有不饱和电子的镍催化剂可以降低氢气的解离能,以克服间歇性氢气供应的缓慢响应,其响应速度(12分钟)比裸氧化物催化剂(42分钟)更快。此外,镍的引入增强了催化剂对氢气的敏感性,得到了一种在较低氢气浓度下具有良好性能的镍/氧化铟催化剂,其对氢气波动范围的适应性是氧化铟的15倍,大大降低了可再生能源产生的不稳定氢气供应的负面影响。