The electrochemical CO_(2) reduction reaction(CO_(2)RR)holds significant promise in advancing carbon neutrality.Developing catalysts for the electrochemical CO_(2)RR to multi-carbon(C_(2+))products(e.g.,C_(2)H_(4))und...The electrochemical CO_(2) reduction reaction(CO_(2)RR)holds significant promise in advancing carbon neutrality.Developing catalysts for the electrochemical CO_(2)RR to multi-carbon(C_(2+))products(e.g.,C_(2)H_(4))under industrial-level current density is urgently needed and pivotal.Herein,we report the Cu_(2)O nanoparticles doped with interstitial carbon atoms(denoted as C-Cu_(2)O NPs)for the conversion of CO_(2) to C_(2+)products.The interstitial carbon promotes the C-Cu_(2)O NPs to possess abundant unsaturated Cu–O bonds,leading to a high-density Cu^(δ+)(0<δ<1)species.The obtained C-Cu_(2)O NPs exhibited significant Faradic efficiency(FE)of C_(2+) products approaching 76.9%and a partial current density reaching 615.2 mA·cm^(–2)under an industrial-level current density of 800 mA·cm^(–2).Furthermore,the efficient electrosynthesis of C_(2)H_(4) achieved an FE of 57.4%with a partial current density of 459.2 mA·cm^(–2).In situ electrochemical attenuated total reflection Fourier transform infrared spectroscopy and in situ Raman spectroscopy analyses revealed that C-Cu_(2)O NPs stabilized the intermediate*CO and facilitated C–C coupling,leading to increased selectivity towards C_(2+) products.展开更多
Anovel metal-organic framework{[In_(3)(TATAT)_(2)]·3CH_(3)NH_(3)·7NMF·8H_(2)O}[JLU-MOF101,H_(6)TATAT=5,5′,5″-(1,3,5-triazine-2,4,6-triyl)tris-(azanediyl)triisophthalate,NMF=N-methyl-formamide]with cor...Anovel metal-organic framework{[In_(3)(TATAT)_(2)]·3CH_(3)NH_(3)·7NMF·8H_(2)O}[JLU-MOF101,H_(6)TATAT=5,5′,5″-(1,3,5-triazine-2,4,6-triyl)tris-(azanediyl)triisophthalate,NMF=N-methyl-formamide]with cor topology has been synthesized under solvothermal conditions.The framework of JLU-MOF101 is constructed by{In(COO)_(4)}-nodes and a hexacarboxylic organic ligand.JLU-MOF101 exhibits excellent fluorescence properties in N,N-dimethylformamide(DMF)solution,and its emission spectrum can be greatly overlapped with the ultraviolet absorption spectra of trinitrophenol(TNP)and 2,4-dinitrophenol(2,4-DNP).As a result,JLU-MOF101 exhibits excellent performance of fluorescence quenching for TNP and 2,4-DNP.In addition,we demonstrate the selective detection capability of JLU-MOF101 through a large number of anti-interference tests.展开更多
Metal-organic frameworks(MOFs) are a class of porous inorganic-organic hybrid materials, which are constructed from diverse inorganic building units and multi-functional organic ligands. Highly ordered pore structures...Metal-organic frameworks(MOFs) are a class of porous inorganic-organic hybrid materials, which are constructed from diverse inorganic building units and multi-functional organic ligands. Highly ordered pore structures and tailored functionalization have made MOF materials potential for applications in many fields. Among various MOF materials, 3p-block metal(Al, Ga, and In)-based MOFs exhibit higher chemical stability than divalent transition metal-based MOFs due to their higher valence. In this review, Al-MOFs and In-MOFs were mainly discussed from the perspective of categories of inorganic building blocks, coordination types, and numbers of organic ligands. This review will give intuitive guidance to the design and synthesis of novel 3p-block metal-based MOFs with potential applications.展开更多
基金supported by the National Key R&D Program of China(No.2018YFA0702001)the National Natural Science Foundation of China(Nos.22371268 and 22301287)+4 种基金Fundamental Research Funds for the Central Universities(No.WK2060000016)Anhui Provincial Natural Science Foundation(Nos.2208085J09 and 2208085QB33)Collaborative Innovation Program of Hefei Science Center,CAS(No.2022HSC-CIP020)Youth Innovation Promotion Association of the Chinese Academy of Science(No.2018494)USTC Tang Scholar.
文摘The electrochemical CO_(2) reduction reaction(CO_(2)RR)holds significant promise in advancing carbon neutrality.Developing catalysts for the electrochemical CO_(2)RR to multi-carbon(C_(2+))products(e.g.,C_(2)H_(4))under industrial-level current density is urgently needed and pivotal.Herein,we report the Cu_(2)O nanoparticles doped with interstitial carbon atoms(denoted as C-Cu_(2)O NPs)for the conversion of CO_(2) to C_(2+)products.The interstitial carbon promotes the C-Cu_(2)O NPs to possess abundant unsaturated Cu–O bonds,leading to a high-density Cu^(δ+)(0<δ<1)species.The obtained C-Cu_(2)O NPs exhibited significant Faradic efficiency(FE)of C_(2+) products approaching 76.9%and a partial current density reaching 615.2 mA·cm^(–2)under an industrial-level current density of 800 mA·cm^(–2).Furthermore,the efficient electrosynthesis of C_(2)H_(4) achieved an FE of 57.4%with a partial current density of 459.2 mA·cm^(–2).In situ electrochemical attenuated total reflection Fourier transform infrared spectroscopy and in situ Raman spectroscopy analyses revealed that C-Cu_(2)O NPs stabilized the intermediate*CO and facilitated C–C coupling,leading to increased selectivity towards C_(2+) products.
基金supported by the National Natural Science Foundation of China(Nos.22171100,22288101)and the“111”Project of China(No.B17020).
文摘Anovel metal-organic framework{[In_(3)(TATAT)_(2)]·3CH_(3)NH_(3)·7NMF·8H_(2)O}[JLU-MOF101,H_(6)TATAT=5,5′,5″-(1,3,5-triazine-2,4,6-triyl)tris-(azanediyl)triisophthalate,NMF=N-methyl-formamide]with cor topology has been synthesized under solvothermal conditions.The framework of JLU-MOF101 is constructed by{In(COO)_(4)}-nodes and a hexacarboxylic organic ligand.JLU-MOF101 exhibits excellent fluorescence properties in N,N-dimethylformamide(DMF)solution,and its emission spectrum can be greatly overlapped with the ultraviolet absorption spectra of trinitrophenol(TNP)and 2,4-dinitrophenol(2,4-DNP).As a result,JLU-MOF101 exhibits excellent performance of fluorescence quenching for TNP and 2,4-DNP.In addition,we demonstrate the selective detection capability of JLU-MOF101 through a large number of anti-interference tests.
基金This work was supported by the National Natural Science Foundation of China(No. 21771078).
文摘Metal-organic frameworks(MOFs) are a class of porous inorganic-organic hybrid materials, which are constructed from diverse inorganic building units and multi-functional organic ligands. Highly ordered pore structures and tailored functionalization have made MOF materials potential for applications in many fields. Among various MOF materials, 3p-block metal(Al, Ga, and In)-based MOFs exhibit higher chemical stability than divalent transition metal-based MOFs due to their higher valence. In this review, Al-MOFs and In-MOFs were mainly discussed from the perspective of categories of inorganic building blocks, coordination types, and numbers of organic ligands. This review will give intuitive guidance to the design and synthesis of novel 3p-block metal-based MOFs with potential applications.
