Electrochemical reduction of CO_(2) to formic acid(HCOOH)is an important route for storing renewable energy and achieving carbon neutrality.Herein,we propose the continuous production of HCOOH solution from electrocat...Electrochemical reduction of CO_(2) to formic acid(HCOOH)is an important route for storing renewable energy and achieving carbon neutrality.Herein,we propose the continuous production of HCOOH solution from electrocatalytic CO_(2) reduction using highly mesoporous bismuth oxide(Bi_(2)O_(3))nanosheets as an electrocatalyst and membrane electrode assembly with solid-state electrolyte as an electrolyzer.Precisely,0.1 M of HCOOH solution could be produced continuously at a current density of -56 mA cm^(-2) for at least 43 h.The underlying mechanism for the high performance of the electrocatalytic system was investigated by experimental studies and theoretical calculations.展开更多
To develop high-performance metal-organic frameworks(MOFs)for catalysis is of great importance.Here,we synthesized the mesoporous Cu_(3−x)Zn_(x)(BTC)_(2)(BTC=benzene-1,3,5-tricarboxylate)nanocubes in a deep eutectic s...To develop high-performance metal-organic frameworks(MOFs)for catalysis is of great importance.Here,we synthesized the mesoporous Cu_(3−x)Zn_(x)(BTC)_(2)(BTC=benzene-1,3,5-tricarboxylate)nanocubes in a deep eutectic solvent of ZnCl_(2)/ethylene glycol solution.The route can proceed at room temperature and the reaction time needed is shortened to be 30 min,which is superior to the conventional solvothermal route that usually needs high temperature and long reaction time.The formation mechanism of the mesoporous Cu_(3−x)Zn_(x)(BTC)_(2)nanocubes in deep eutectic solvent(DES)was investigated by in situ synchrotron X-ray diffraction/small angle X-ray scattering/X-ray absorption fine structure conjunction technique.The mesoporous Cu_(3−x)Zn_(x)(BTC)_(2)nanocubes exhibit high catalytic activity and reusability for cyanosilylation reaction of benzaldehyde and aerobic oxidation reaction of benzylic alcohol.展开更多
To improve the electrocatalytic conversion of carbon dioxide(CO_(2))into C_(2+)products(such as ethylene(C_(2)H_(4))and ethanol(CH_(3)CH_(2)OH),etc.)is of great importance,but remains challenging.Herein,we proposed a ...To improve the electrocatalytic conversion of carbon dioxide(CO_(2))into C_(2+)products(such as ethylene(C_(2)H_(4))and ethanol(CH_(3)CH_(2)OH),etc.)is of great importance,but remains challenging.Herein,we proposed a strategy that directs the C–C coupling pathway through enriching and confining the carbon monoxide(CO)intermediate to internal pores of Cu nanocubes,for electrocatalytic reduction of CO_(2)into C_(2+)chemicals.In H-type cell,the Faraday efficiency(FE)for ethylene and ethanol reaches 70.3%at−1.28 V versus the reversible hydrogen electrode(vs.RHE),with a current density of 47.9 mA·cm^(−2).In flow cell,the total current density is up to 340.3 mA·cm^(−2)at^(−2).38 V(vs.RHE)and the FE for C_(2+)products is 67.4%.Experimental and theoretical studies reveal that both the CO intermediate adsorption and C–C coupling reaction on such an internal porous catalyst are facilitated,thus improving CO_(2)-to-C_(2+)conversion efficiency.展开更多
Ultrathin two-dimensional （2D） porous Zn（OH）2 nanosheets （PNs） were fabricated by means of one-dimensional Cu nanowires as backbones. The PNs have thickness of approximately 3.8 nm and pore size of 4-10 nm. To f...Ultrathin two-dimensional （2D） porous Zn（OH）2 nanosheets （PNs） were fabricated by means of one-dimensional Cu nanowires as backbones. The PNs have thickness of approximately 3.8 nm and pore size of 4-10 nm. To form ＂smart＂ porous nanosheets, DNA aptamers were covalently conjugated to the surface of PNs. These ultrathin nanosheets show good biocompatibility, effident cellular uptaker and promising pH-stimulated drug release.展开更多
基金supported by the National Natural Science Foundation of China(grant nos.22033009,22121002,and 22238011).
文摘Electrochemical reduction of CO_(2) to formic acid(HCOOH)is an important route for storing renewable energy and achieving carbon neutrality.Herein,we propose the continuous production of HCOOH solution from electrocatalytic CO_(2) reduction using highly mesoporous bismuth oxide(Bi_(2)O_(3))nanosheets as an electrocatalyst and membrane electrode assembly with solid-state electrolyte as an electrolyzer.Precisely,0.1 M of HCOOH solution could be produced continuously at a current density of -56 mA cm^(-2) for at least 43 h.The underlying mechanism for the high performance of the electrocatalytic system was investigated by experimental studies and theoretical calculations.
基金support by Ministry of Science and Technology of China(No.2017YFA0403003)the National Natural Science Foundation of China(Nos.22033009 and 22121002).
文摘To develop high-performance metal-organic frameworks(MOFs)for catalysis is of great importance.Here,we synthesized the mesoporous Cu_(3−x)Zn_(x)(BTC)_(2)(BTC=benzene-1,3,5-tricarboxylate)nanocubes in a deep eutectic solvent of ZnCl_(2)/ethylene glycol solution.The route can proceed at room temperature and the reaction time needed is shortened to be 30 min,which is superior to the conventional solvothermal route that usually needs high temperature and long reaction time.The formation mechanism of the mesoporous Cu_(3−x)Zn_(x)(BTC)_(2)nanocubes in deep eutectic solvent(DES)was investigated by in situ synchrotron X-ray diffraction/small angle X-ray scattering/X-ray absorption fine structure conjunction technique.The mesoporous Cu_(3−x)Zn_(x)(BTC)_(2)nanocubes exhibit high catalytic activity and reusability for cyanosilylation reaction of benzaldehyde and aerobic oxidation reaction of benzylic alcohol.
基金supported by the National Natural Science Foundation of China(Nos.22033009 and 22121002).
文摘To improve the electrocatalytic conversion of carbon dioxide(CO_(2))into C_(2+)products(such as ethylene(C_(2)H_(4))and ethanol(CH_(3)CH_(2)OH),etc.)is of great importance,but remains challenging.Herein,we proposed a strategy that directs the C–C coupling pathway through enriching and confining the carbon monoxide(CO)intermediate to internal pores of Cu nanocubes,for electrocatalytic reduction of CO_(2)into C_(2+)chemicals.In H-type cell,the Faraday efficiency(FE)for ethylene and ethanol reaches 70.3%at−1.28 V versus the reversible hydrogen electrode(vs.RHE),with a current density of 47.9 mA·cm^(−2).In flow cell,the total current density is up to 340.3 mA·cm^(−2)at^(−2).38 V(vs.RHE)and the FE for C_(2+)products is 67.4%.Experimental and theoretical studies reveal that both the CO intermediate adsorption and C–C coupling reaction on such an internal porous catalyst are facilitated,thus improving CO_(2)-to-C_(2+)conversion efficiency.
基金The authors are grateful to Dr. Kathryn Williams for her critical comments during the preparation of this manuscript. This work is supported by grants awarded by the National Institutes of Health （No. GM079359 and CA133086）. This work is also supported by the National Basic Research Program of China （No. 2011CB911000）, National Natural Science Foundation of China （Nos. 21221003 and 21327009） and China National Instrumentation Program （No. 2011YQ03012412）.
文摘Ultrathin two-dimensional （2D） porous Zn（OH）2 nanosheets （PNs） were fabricated by means of one-dimensional Cu nanowires as backbones. The PNs have thickness of approximately 3.8 nm and pore size of 4-10 nm. To form ＂smart＂ porous nanosheets, DNA aptamers were covalently conjugated to the surface of PNs. These ultrathin nanosheets show good biocompatibility, effident cellular uptaker and promising pH-stimulated drug release.
