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同时激活C-C和C-O键以最大限度地利用木质素在InGaN上产生合成气的二元铁锰助催化剂
作者:小柯机器人 发布时间:2024/10/31 22:39:07

上海交通大学黄震团队报道了同时激活C-C和C-O键,以最大限度地利用木质素在InGaN上产生合成气的二元铁锰助催化剂。相关研究成果于2024年10月30日发表在国际知名学术期刊《德国应用化学》。

太阳能木质素重整为合成气生产提供了一条碳中和路线。

该研究探索了一种双非贵铁锰助催化剂,可同时激活C-C和C-O键,以最大限度地利用天然木质素的各种取代基来生产合成气。

通过在硅片上与InGaN纳米线组装,所设计的双FeMn助催化剂可从蒸馏水中的天然木质素中,获得42.4 mol·gcat-1·h-1的可测量合成气释放速率,选择性高达93%,在聚光下H2/CO比可调,导致11.8%的光燃比。

InGaN的一维纳米结构产生的高FeMn原子效率,能够实现每摩尔FeMn每小时220896摩尔合成气的高转换频率(TOF)。

通过相关探索实验,研究人员在原子水平上揭示了双FeMn助催化剂,在木质素和水向合成气演化机制中的关键作用。

研究发现,由InGaN纳米线负载的协同铁锰助催化剂,能够以相当的最小离解能同时激活C-C和C-O键。

该项工作展示了一种新的、地球富含的双功能助催化剂,用于利用木质素的各种取代基,生产由化石燃料以外的阳光驱动的合成气。

附:英文原文

Title: Binary Iron-Manganese Cocatalyst for Simultaneous Activation of C-C and C-O Bonds to Maximally Utilize Lignin for Syngas Generation over InGaN

Author: Baowen Zhou, Tianqi Yu, Ying Zhao, Jingling Li, Yixin Li, Liang Qiu, Hu Pan, Muhammad Salman Nasir, Jun Song, Zhen Huang

Issue&Volume: 2024-10-30

Abstract: Solar-powered lignin reforming offers a carbon-neutral route for syngas production. This study explores a dual non-precious iron-manganese cocatalyst to simultaneously activate both C-C and C-O bonds for maximizing the utilization of various substituents of native lignin to yield syngas. By assembling with InGaN nanowires on a Si wafer, the as-designed dual FeMn cocatalyst affords a measurable syngas evolution rate of 42.4 mol·gcat-1·h-1 from native lignin in distilled water with a high selectivity of 93% and tunable H2/CO ratios under concentrated light, leading to a considerable light-to-fuel efficiency of 11.8%. The high FeMn atom efficiency arising from the 1-dimensional nanostructure of InGaN enables the achievement of a high turnover frequency (TOF) of 220896 mol syngas per mol FeMn per hour. By correlating exploration experiments, the critical role of the dual FeMn cocatalyst in the evolving mechanism of lignin and water toward syngas is disclosed at the atomic level. It is discovered that the synergetic iron-manganese cocatalyst supported by InGaN nanowires enables simultaneous activation of C-C and C-O bonds with comparable minimized dissociation energies. This work demonstrates a new and earth-abundant bifunctional cocatalyst for utilizing various substituents of lignin to produce syngas powered by sunlight beyond fossil fuels.

DOI: 10.1002/anie.202413528

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202413528

期刊信息

Angewandte Chemie:《德国应用化学》,创刊于1887年。隶属于德国化学会,最新IF:16.823
官方网址:https://onlinelibrary.wiley.com/journal/15213773
投稿链接:https://www.editorialmanager.com/anie/default.aspx