Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is chall...Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is challenging because of the inefficient mass transfer of the catalyst and the presence of the hydrogen evolution reaction(HER).In this study,dendritic Cu/Cu_(2)O with abundant Cu^(0)/Cu^(+)interfaces and numerous dendritic curves was synthesized in a CO_(2)atmosphere,resulting in the high selectivity and current density of the C_(2)products.Dendritic Cu/Cu_(2)O achieved a C_(2)Faradaic efficiency of 69.8%and a C_(2)partial current density of 129.5 mA cm^(-2)in an H-cell.Finite element simulations showed that a dendritic structure with a high curvature generates a strong electric field,leading to a localized CO_(2)concentration.Additionally,DRT analysis showed that a dendritic struc-ture with a high curvature actively adsorbed the surrounding high concentration of CO_(2),enhancing the mass transfer rate and achieving a high current density.During the experiment,the impact of the electronic structure on the performance of the catalyst was investigated by varying the atomic ratio of Cu^(0)/Cu^(+) on the catalyst surface,which resulted in improved ethylene selectivity.Under the optimal atomic ratio of Cu^(0)/Cu^(+),the charge transfer resistance was minimized,and the desorption rate of the intermediates was low,favoring C_(2) generation.Density functional theory calculations indicated that the Cu^(0)/Cu^(+) interfaces exhibited a lower Gibbs free energy for the rate-determining step,enhancing C_(2)H_(4) formation.The Cu/Cu_(2)O catalyst also exhibited a low Cu d-band center,which enhanced the adsorption stability of *CO on the surface and facilitated C_(2)formation.This observa-tion explained the higher yield of C_(2) products at the Cu^(0)/Cu^(+) interface than that of H_(2) under rapid mass transfer.The results of the net present value model showed that the H-cell holds promising industrial prospects,contingent upon it being a catalyst with both high selectivity and high current density.This approach of integrating the structure and composition provides new insights for ad-vancing the CO_(2)RR towards high-current C_(2) products.展开更多
Aqueous Zinc-ion batteries(ZIBs),using zinc negative electrode and aqueous electrolyte,have attracted great attention in energy storage field due to the reliable safety and low-cost.A composite material comprised of V...Aqueous Zinc-ion batteries(ZIBs),using zinc negative electrode and aqueous electrolyte,have attracted great attention in energy storage field due to the reliable safety and low-cost.A composite material comprised of VO2·0.2H2O nanocuboids anchored on graphene sheets(VOG)is synthesized through a facile and efficient microwave-assisted solvothermal strategy and is used as aqueous ZIBs cathode material.Owing to the synergistic effects between the high conductivity of graphene sheets and the desirable structural features of VO2·0.2H2O nanocuboids,the VOG electrode has excellent electronic and ionic transport ability,resulting in superior Zn ions storage performance.The Zn/VOG system delivers ultrahigh specific capacity of 423 mAh·g^−1 at 0.25 A·g^−1 and exhibits good cycling stability of up to 1,000 cycles at 8 A·g^−1 with 87%capacity retention.Systematical structural and elemental characterizations confirm that the interlayer space of VO2·0.2H2O nanocuboids can adapt to the reversible Zn ions insertion/extraction.The as-prepared VOG composite is a promising cathode material with remarkable electrochemical performance for low-cost and safe aqueous rechargeable ZIBs.展开更多
The Ag/Mg0.2Zn0.8O/ZnMn2O4/p^＋-Si heterostructure devices were fabricated by sol-gel spin coating technique and the resistive switching behavior,conduction mechanism,endurance characteristic,and retention properties ...The Ag/Mg0.2Zn0.8O/ZnMn2O4/p^＋-Si heterostructure devices were fabricated by sol-gel spin coating technique and the resistive switching behavior,conduction mechanism,endurance characteristic,and retention properties were investigated.A distinct bipolar resistive switching behavior of the devices was observed at room temperature.The resistance ratio R_（HRS）/RLRS of high resistance state and low resistance state is as large as four orders of magnitude with a readout voltage of 2.0 V.The dominant conduction mechanism of the device is trap-controlled space charge limited current（SCLC）.The devices exhibit good durability under 1×10^3cycles and the degradation is invisible for more than 10^6 s.展开更多
A new compound 2 6[Co(H 2O) 2(VO) 8(OH) 4(PO 4) 8] has been hydrothermally synthesized. Single crystal X-ray analysis indicates that this compound crystallizes in a monoclinic system, space group P2 1/n with a=1.438 5...A new compound 2 6[Co(H 2O) 2(VO) 8(OH) 4(PO 4) 8] has been hydrothermally synthesized. Single crystal X-ray analysis indicates that this compound crystallizes in a monoclinic system, space group P2 1/n with a=1.438 5(3) nm, b=1.012 2(2) nm, c=1.832 5(4) nm, β=90.21°, V=2\^668 2(9) nm 3, Z=2, D c=2.112 g/cm 3, R=0.055, wR=0.149 7, S=1.037. The structure of 2 6[Co(H 2O) 2(VO) 8(OH) 4(PO 4) 8] is characterized by P-V-O layers constructed by [(VO) 4(OH) 2(PO 4) 4] 6- non-symmetric units. The P-V-O layers are pillared by [Co(H 2O) 2] 2+ group, resulting in the channels within which the protonated diaminoethane and H 3O + are located.展开更多
文摘Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is challenging because of the inefficient mass transfer of the catalyst and the presence of the hydrogen evolution reaction(HER).In this study,dendritic Cu/Cu_(2)O with abundant Cu^(0)/Cu^(+)interfaces and numerous dendritic curves was synthesized in a CO_(2)atmosphere,resulting in the high selectivity and current density of the C_(2)products.Dendritic Cu/Cu_(2)O achieved a C_(2)Faradaic efficiency of 69.8%and a C_(2)partial current density of 129.5 mA cm^(-2)in an H-cell.Finite element simulations showed that a dendritic structure with a high curvature generates a strong electric field,leading to a localized CO_(2)concentration.Additionally,DRT analysis showed that a dendritic struc-ture with a high curvature actively adsorbed the surrounding high concentration of CO_(2),enhancing the mass transfer rate and achieving a high current density.During the experiment,the impact of the electronic structure on the performance of the catalyst was investigated by varying the atomic ratio of Cu^(0)/Cu^(+) on the catalyst surface,which resulted in improved ethylene selectivity.Under the optimal atomic ratio of Cu^(0)/Cu^(+),the charge transfer resistance was minimized,and the desorption rate of the intermediates was low,favoring C_(2) generation.Density functional theory calculations indicated that the Cu^(0)/Cu^(+) interfaces exhibited a lower Gibbs free energy for the rate-determining step,enhancing C_(2)H_(4) formation.The Cu/Cu_(2)O catalyst also exhibited a low Cu d-band center,which enhanced the adsorption stability of *CO on the surface and facilitated C_(2)formation.This observa-tion explained the higher yield of C_(2) products at the Cu^(0)/Cu^(+) interface than that of H_(2) under rapid mass transfer.The results of the net present value model showed that the H-cell holds promising industrial prospects,contingent upon it being a catalyst with both high selectivity and high current density.This approach of integrating the structure and composition provides new insights for ad-vancing the CO_(2)RR towards high-current C_(2) products.
基金The authors are thankful to funds from the China Postdoctoral Science Foundation(No.RZ1900011127)Qingdao Innovation Leading Talent Program and Taishan Scholars Program and Natural Science Foundation of Shandong(No.ZR2017BEM028)+4 种基金M.S.is thankful to funds from the Science Foundation of Jiangsu Province(No.BK20171169)C.W.L.thanks the support from National Natural Science Foundation of China(No.51802168)China Postdoctoral Science Foundation(No.2018M630753)Natural Science Foundation of Shandong Province(No.ZR2018BEM006)Qingdao Postdoctoral Application Research Project.
文摘Aqueous Zinc-ion batteries(ZIBs),using zinc negative electrode and aqueous electrolyte,have attracted great attention in energy storage field due to the reliable safety and low-cost.A composite material comprised of VO2·0.2H2O nanocuboids anchored on graphene sheets(VOG)is synthesized through a facile and efficient microwave-assisted solvothermal strategy and is used as aqueous ZIBs cathode material.Owing to the synergistic effects between the high conductivity of graphene sheets and the desirable structural features of VO2·0.2H2O nanocuboids,the VOG electrode has excellent electronic and ionic transport ability,resulting in superior Zn ions storage performance.The Zn/VOG system delivers ultrahigh specific capacity of 423 mAh·g^−1 at 0.25 A·g^−1 and exhibits good cycling stability of up to 1,000 cycles at 8 A·g^−1 with 87%capacity retention.Systematical structural and elemental characterizations confirm that the interlayer space of VO2·0.2H2O nanocuboids can adapt to the reversible Zn ions insertion/extraction.The as-prepared VOG composite is a promising cathode material with remarkable electrochemical performance for low-cost and safe aqueous rechargeable ZIBs.
基金Funded by the National Natural Science Foundation of China(No.51262003)the Guangxi Key Laboratory of Information Materials(Guilin University of Electronic Technology),China(No.1110908-10-Z)
文摘The Ag/Mg0.2Zn0.8O/ZnMn2O4/p^＋-Si heterostructure devices were fabricated by sol-gel spin coating technique and the resistive switching behavior,conduction mechanism,endurance characteristic,and retention properties were investigated.A distinct bipolar resistive switching behavior of the devices was observed at room temperature.The resistance ratio R_（HRS）/RLRS of high resistance state and low resistance state is as large as four orders of magnitude with a readout voltage of 2.0 V.The dominant conduction mechanism of the device is trap-controlled space charge limited current（SCLC）.The devices exhibit good durability under 1×10^3cycles and the degradation is invisible for more than 10^6 s.
文摘以磷钼钒杂多酸H4PMo11V1O40为催化剂、乙酸为溶剂,用双氧水氧化2-甲基萘制备2-甲基萘醌.实验表明：H4PMo11V1O40具有一定的催化活性.通过正交试验和单因素试验考察了催化剂用量、乙酸用量、双氧水用量、反应时间、反应温度等对收率的影响,获得较佳的合成条件：杂多酸∶2-MN（质量比）=7%,乙酸∶2-MN（质量比）=10.5∶1,双氧水∶2-甲基萘（摩尔比）=4.2∶1,较适宜的温度为40~50℃,反应时间为30 min.
文摘A new compound 2 6[Co(H 2O) 2(VO) 8(OH) 4(PO 4) 8] has been hydrothermally synthesized. Single crystal X-ray analysis indicates that this compound crystallizes in a monoclinic system, space group P2 1/n with a=1.438 5(3) nm, b=1.012 2(2) nm, c=1.832 5(4) nm, β=90.21°, V=2\^668 2(9) nm 3, Z=2, D c=2.112 g/cm 3, R=0.055, wR=0.149 7, S=1.037. The structure of 2 6[Co(H 2O) 2(VO) 8(OH) 4(PO 4) 8] is characterized by P-V-O layers constructed by [(VO) 4(OH) 2(PO 4) 4] 6- non-symmetric units. The P-V-O layers are pillared by [Co(H 2O) 2] 2+ group, resulting in the channels within which the protonated diaminoethane and H 3O + are located.
