Electrocatalytic Biomass Upgrading of Furfural using Transition-Metal Borides via Density Functional Theory Investigation.
Electrocatalytic Biomass Upgrading of Furfural using Transition-Metal Borides via Density Functional Theory Investigation.
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DOI：
10.1002/smll.202205876
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发表时间：
2022-12
期刊：
影响因子：
13.3
通讯作者：
Yi Xiao;Chen Shen;Weibin Zhang;Meiling Zhang;Haotong Zhang;Taihuan Shao;Zhengwei Xiong;Yingchun Ding;Shu Hao;Li Liu;Yuan Chen;Jinyang Li
中科院分区：
文献类型：
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作者：
Yi Xiao;Chen Shen;Weibin Zhang;Meiling Zhang;Haotong Zhang;Taihuan Shao;Zhengwei Xiong;Yingchun Ding;Shu Hao;Li Liu;Yuan Chen;Jinyang Li
电催化生物质升级已被证明是一种产生增值产品的有效技术。本文介绍了过渡金属硼化物（MBenes）用于糠醛改质同时制氢的设计和开发。利用密度泛函理论，系统评价了13种候选MBene的稳定性、选择性和活性，用于糠醛改质。结果表明，Fe_2B_2对糠酸（FAC）和5-羟基-2（5 H）-呋喃酮（HFO）的生成具有良好的电催化活性，其极限电位分别为-0.15V和-0.93V。此外，Fe_2B_2和Mn_2Fe_2的极限电位分别为-1.35和-1.36V。用于制备6-羟基-2，3-二氢-6H-吡喃-3-酮（HDPO），表明它们也可以用作电催化剂。根据Sabatier原理，提出了一种用于筛选高催化活性催化剂的材料性质描述符（φ），该描述符考虑了金属的电负性和d电子数。此外，表面氧化还原电位，电子性质，和电荷密度差确定为Fe 2 B2，这是估计表现出高的催化活性，糠醛氧化为FAC和HFO。
Electrocatalytic biomass upgrading has proven to be an effective technique for generating value-added products. Herein, the design and development of furfural upgrading using transition-metal borides (MBenes) with simultaneous production of hydrogen are presented. Using density functional theory, the stabilities, selectivities, and activities of 13 MBene candidates are systematically evaluated for furfural upgrading. This research suggests that Fe2 B2 can serve as a promising electrocatalyst for the formation of furoic acid (FAC), with a limiting potential of -0.15 V, and 5-hydroxy-2(5H)-furanone (HFO), with a limiting potential of -0.93 V. Furthermore, Fe2 B2 and Mn2 Fe2 are shown to exhibit favorable limiting potentials of -1.35 and -1.36 V, respectively, for producing 6-hydroxy-2.3-dihydro-6H-pyrano-3-one (HDPO), indicating that they may also serve as electrocatalysts. Based on Sabatier's principle, a descriptor (φ) of material properties is developed for screening catalysts with high catalytic activity considering the electronegativities and d-electron number of metals. Additionally, surface redox potential, electronic properties, and charge-density differences are determined for Fe2 B2 , which is estimated to exhibit high catalytic activity for the oxidation of furfural to FAC and HFO.