金属–载体相互作用不仅调控金属的电子结构,还可以稳定金属纳米颗粒,被认为是一种提高电解水析氢反应性能的有效策略。本文采用4,4’-联吡啶与Cs2[closo-B12H12]为前驱体,通过静电组装制备了新型硼有机聚合物(BOPs),并以此作为还原剂...金属–载体相互作用不仅调控金属的电子结构,还可以稳定金属纳米颗粒,被认为是一种提高电解水析氢反应性能的有效策略。本文采用4,4’-联吡啶与Cs2[closo-B12H12]为前驱体,通过静电组装制备了新型硼有机聚合物(BOPs),并以此作为还原剂和载体,原位还原–煅烧两步法制备硼氮双掺杂碳载体负载钌纳米颗粒催化剂(Ru/BCN)。主要探究了合成过程中不同煅烧温度对于Ru/BCN的HER性能的影响,研究发现Ru/BCN-700展现出最佳的析氢活性,在碱性介质中仅需要17 mV的过电位就可达到10 mA cm−2的电流密度,并且具有良好的稳定性和耐久性。展开更多
Constructed by selecting appropriate building blocks,covalent organic frameworks(COFs)can be endowed with a variety of specific functions.Herein,we successfully synthesized an imine‐linked H_(2)PReBpy‐COF with the C...Constructed by selecting appropriate building blocks,covalent organic frameworks(COFs)can be endowed with a variety of specific functions.Herein,we successfully synthesized an imine‐linked H_(2)PReBpy‐COF with the CO_(2) reduction catalyst[ReI(bpy)(CO)_(3)Cl]and the porphyrin photosensitizer as the monomeric building units.The light‐harvesting properties of the porphyrin itself,augmented by the extendedπ‐conjugated planar structure of 2D COF,enable H_(2)PReBpy‐COF the excellent light‐harvesting capability,efficient charge separation,and fast interfacial charge transfer.In addition,a large amount of uniformly distributed[ReI(bpy)(CO)_(3)Cl]units offer H_(2)PReBpy‐COF an excellent activity toward photocatalytic CO_(2) reduction with moderate selectivity and reusability.This study demonstrated a proof of concept in which the advantages of COFs and functional monomers are rationally integrated for photocatalytic solar fuel conversion.展开更多
A pseudorotaxane of cucurbit[6]uril (CB[6]) with guest molecule N,N'-hexamethylenebis (pyrazinyl perehlorate) (BPHP) was synthesized and characterized by IH NMR spectra, IR, single crystal X-ray diffraction ana...A pseudorotaxane of cucurbit[6]uril (CB[6]) with guest molecule N,N'-hexamethylenebis (pyrazinyl perehlorate) (BPHP) was synthesized and characterized by IH NMR spectra, IR, single crystal X-ray diffraction analysis and thermogravimetric analysis. The structure of the pseudorotaxane (CB[6]BPHP) is stabilized by host-guest hydro- gen bonds. Self-assembly of the pseudorotaxane produces infinite one-dimensional and two-dimensional networks with intermolecular hydrogen bonds. In the molecular packing of the CB[6].BPHP, C104(H20)2 water clusters serve as bridges to associate these pseudorotaxanes and form three-dimensional networked pseudopolyrotaxane.展开更多
文摘金属–载体相互作用不仅调控金属的电子结构,还可以稳定金属纳米颗粒,被认为是一种提高电解水析氢反应性能的有效策略。本文采用4,4’-联吡啶与Cs2[closo-B12H12]为前驱体,通过静电组装制备了新型硼有机聚合物(BOPs),并以此作为还原剂和载体,原位还原–煅烧两步法制备硼氮双掺杂碳载体负载钌纳米颗粒催化剂(Ru/BCN)。主要探究了合成过程中不同煅烧温度对于Ru/BCN的HER性能的影响,研究发现Ru/BCN-700展现出最佳的析氢活性,在碱性介质中仅需要17 mV的过电位就可达到10 mA cm−2的电流密度,并且具有良好的稳定性和耐久性。
文摘Constructed by selecting appropriate building blocks,covalent organic frameworks(COFs)can be endowed with a variety of specific functions.Herein,we successfully synthesized an imine‐linked H_(2)PReBpy‐COF with the CO_(2) reduction catalyst[ReI(bpy)(CO)_(3)Cl]and the porphyrin photosensitizer as the monomeric building units.The light‐harvesting properties of the porphyrin itself,augmented by the extendedπ‐conjugated planar structure of 2D COF,enable H_(2)PReBpy‐COF the excellent light‐harvesting capability,efficient charge separation,and fast interfacial charge transfer.In addition,a large amount of uniformly distributed[ReI(bpy)(CO)_(3)Cl]units offer H_(2)PReBpy‐COF an excellent activity toward photocatalytic CO_(2) reduction with moderate selectivity and reusability.This study demonstrated a proof of concept in which the advantages of COFs and functional monomers are rationally integrated for photocatalytic solar fuel conversion.
文摘A pseudorotaxane of cucurbit[6]uril (CB[6]) with guest molecule N,N'-hexamethylenebis (pyrazinyl perehlorate) (BPHP) was synthesized and characterized by IH NMR spectra, IR, single crystal X-ray diffraction analysis and thermogravimetric analysis. The structure of the pseudorotaxane (CB[6]BPHP) is stabilized by host-guest hydro- gen bonds. Self-assembly of the pseudorotaxane produces infinite one-dimensional and two-dimensional networks with intermolecular hydrogen bonds. In the molecular packing of the CB[6].BPHP, C104(H20)2 water clusters serve as bridges to associate these pseudorotaxanes and form three-dimensional networked pseudopolyrotaxane.