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Porous Bimetallic Ti-MOFs for Photocatalytic Oxidation of Amines in Air
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2024-10-01 , DOI: 10.1021/acs.inorgchem.4c03381
Xiaoying Zhang, Xuze Pan, Xuezhen Si, Laiyang Zhu, Qingxia Yao, Wenzeng Duan, Xianqiang Huang, Jie Su
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2024-10-01 , DOI: 10.1021/acs.inorgchem.4c03381
Xiaoying Zhang, Xuze Pan, Xuezhen Si, Laiyang Zhu, Qingxia Yao, Wenzeng Duan, Xianqiang Huang, Jie Su
A family of microporous titanium-containing metal–organic frameworks (denoted as M2Ti-CPCDC, M = Mn, Co, Ni) has been synthesized by using a bimetallic [M2Ti(μ3-O)(COO)6] cluster and a tritopic carbazole-based organic ligand H3CPCDC. M2Ti-CPCDC are stable and display permanent porosity for N2 and CO2 uptake, ranking among the most porous titanium-based metal–organic frameworks. M2Ti-CPCDC crystals exhibit n-type semiconductor behavior. Further catalytic studies demonstrate that all M2Ti-CPCDC materials are applicable for triggering photo-oxidative reactions of amines in air. More specifically, amines with electron-donating groups afford the aldehydes as the main products, while amines bearing electron-withdrawing groups give rise to imines as the main product. Among them, Mn2Ti-CPCDC exhibit the best photocatalytic activity, with conversion of benzylamine up to 99% and selectivity of 99%. Mn2Ti-CPCDC could be recycled in at least three runs while retaining crystallinity and catalytic activity. The reaction mechanism indicates that photoinduced hole (h+), superoxide radical anion (O2·–), and singlet oxygen (1O2) are the main active species involved in the photo-oxidation process.
中文翻译:
多孔双金属 Ti-MOF 用于空气中胺类的光催化氧化
通过使用双金属 [M2Ti(μ3-O)(COO)6] 簇和三位咔唑基有机配体 H3CPCDC,合成了一族微孔含钛金属有机框架(表示为 M2Ti-CPCDC、M = Mn、Co、Ni)。M2Ti-CPCDC 很稳定,对 N2 和 CO2 的吸收显示出永久的孔隙率,是孔隙率最高的钛基金属有机框架之一。M2Ti-CPCDC 晶体表现出 n 型半导体行为。进一步的催化研究表明,所有 M2Ti-CPCDC 材料都适用于在空气中触发胺的光氧化反应。更具体地说,带有供电子基团的胺以醛为主要产物,而带有吸电子基团的胺以亚胺为主要产物。其中,Mn2Ti-CPCDC 表现出最佳的光催化活性,苄胺转化率高达 99%,选择性为 99%。Mn2Ti-CPCDC 可以在至少三次运行中回收,同时保持结晶度和催化活性。反应机理表明,光诱导空穴 (h+)、超氧自由基阴离子 (O2·–) 和单线态氧 (1O2) 是参与光氧化过程的主要活性物质。
更新日期:2024-10-01
中文翻译:
多孔双金属 Ti-MOF 用于空气中胺类的光催化氧化
通过使用双金属 [M2Ti(μ3-O)(COO)6] 簇和三位咔唑基有机配体 H3CPCDC,合成了一族微孔含钛金属有机框架(表示为 M2Ti-CPCDC、M = Mn、Co、Ni)。M2Ti-CPCDC 很稳定,对 N2 和 CO2 的吸收显示出永久的孔隙率,是孔隙率最高的钛基金属有机框架之一。M2Ti-CPCDC 晶体表现出 n 型半导体行为。进一步的催化研究表明,所有 M2Ti-CPCDC 材料都适用于在空气中触发胺的光氧化反应。更具体地说,带有供电子基团的胺以醛为主要产物,而带有吸电子基团的胺以亚胺为主要产物。其中,Mn2Ti-CPCDC 表现出最佳的光催化活性,苄胺转化率高达 99%,选择性为 99%。Mn2Ti-CPCDC 可以在至少三次运行中回收,同时保持结晶度和催化活性。反应机理表明,光诱导空穴 (h+)、超氧自由基阴离子 (O2·–) 和单线态氧 (1O2) 是参与光氧化过程的主要活性物质。