In this study, the solar thermochemical reactor performance for CO_2 utilization into synthesis gas(H_2+ CO) based on CH_4 reforming process was investigated in the context of carbon capture and utilization(CCU) techn...In this study, the solar thermochemical reactor performance for CO_2 utilization into synthesis gas(H_2+ CO) based on CH_4 reforming process was investigated in the context of carbon capture and utilization(CCU) technologies. The P1 radiation heat transfer model is adopted to establish the heat and mass transfer model coupled with thermochemical reaction kinetics. The reactor thermal behavior with direct heat transfer between gaseous reactant and products evolution and the effects of different structural parameters were evaluated. It was found that the reactor has the potential to utilize by ～60% of CO_2 captured with 40% of CH_4 co-fed into syngas(72.9% of H_2 and 27.1% of CO) at 741.31 k W/mof incident radiation heat flux. However, the solar irradiance heat flux and temperature distribution were found to significantly affect the reactant species conversion efficiency and syngas production. The chemical reaction is mainly driven by the thermal energy and higher species conversion into syngas was observed when the temperature distribution at the inner cavity of the reactor was more uniform. Designed a solar thermochemical reactor able to volumetric store concentrated irradiance could highly improve CCU technologies for producing energy-rich chemicals. Besides, the mixture gas inlet velocity, operating pressure and CO_2/CH_4 feeding ratio were crucial to determining the efficiency of CO_2 utilization to solar fuels. Catalytic CO_2-reforming of CH_4 to chemical energy is a promising strategy for an efficient utilization of CO_2 as a renewable carbon source.展开更多
The exploration of sustainable energy utilization requires the imple-mentation of advanced electrochemical devices for efficient energy conversion and storage,which are enabled by the usage of cost-effective,high-perf...The exploration of sustainable energy utilization requires the imple-mentation of advanced electrochemical devices for efficient energy conversion and storage,which are enabled by the usage of cost-effective,high-performance electro-catalysts.Currently,heterogeneous atomically dispersed catalysts are considered as potential candidates for a wide range of applications.Compared to conventional cata-lysts,atomically dispersed metal atoms in carbon-based catalysts have more unsatu-rated coordination sites,quantum size effect,and strong metal-support interactions,resulting in exceptional catalytic activity.Of these,dual-atomic catalysts(DACs)have attracted extensive attention due to the additional synergistic effect between two adja-cent metal atoms.DACs have the advantages of full active site exposure,high selectiv-ity,theoretical 100%atom utilization,and the ability to break the scaling relationship of adsorption free energy on active sites.In this review,we summarize recent research advancement of DACs,which includes(1)the comprehensive understanding of the synergy between atomic pairs;(2)the synthesis of DACs;(3)characterization meth-ods,especially aberration-corrected scanning transmission electron microscopy and synchrotron spectroscopy;and(4)electrochemical energy-related applications.The last part focuses on great potential for the electrochemical catalysis of energy-related small molecules,such as oxygen reduction reaction,CO_(2) reduction reaction,hydrogen evolution reaction,and N_(2) reduction reaction.The future research challenges and opportunities are also raised in prospective section.展开更多
Reducing the anthropogenic COemissions from fossil resource combustion and human activities has become one of the major challenges we are facing today.Beyond those practical applications for the utilization of CO,such...Reducing the anthropogenic COemissions from fossil resource combustion and human activities has become one of the major challenges we are facing today.Beyond those practical applications for the utilization of CO,such as the synthesis of salicylic acid,methanol,urea,NaHCO-NaCOchemicals and recently developed polycarbonate synthesis,scientists are still seeking new materials and technologies for efficient capture,展开更多
To improve the electrocatalytic transformation of carbon dioxide (CO_(2)) to multi-carbon (C_(2+)) products is of great importance.Here we developed a nitrogen-doped Cu catalyst,by which the maximum C_(2+) Faradaic ef...To improve the electrocatalytic transformation of carbon dioxide (CO_(2)) to multi-carbon (C_(2+)) products is of great importance.Here we developed a nitrogen-doped Cu catalyst,by which the maximum C_(2+) Faradaic efficiency can reach 72.7%in flow-cell system,with the partial current density reaching 0.62 A cm^(-2).The in situ Raman spectra demonstrate that the *CO adsorption can be strengthened on such a N-doped Cu catalyst,thus promoting the *CO utilization in the subsequent C–C coupling step.Simultaneously,the water activation can be well enhanced by N doping on Cu catalyst.Owing to the synergistic effects,the selectivity and activity for C_(2+) products over the N-deoped Cu catalyst are much improved.展开更多
基金supported by the National Natural Science Foundation of China (No. 51522601)Chang Jiang Young Scholars Program of China (Q2016186)the Fok Ying Tong Education Foundation of China (No. 141055)
文摘In this study, the solar thermochemical reactor performance for CO_2 utilization into synthesis gas(H_2+ CO) based on CH_4 reforming process was investigated in the context of carbon capture and utilization(CCU) technologies. The P1 radiation heat transfer model is adopted to establish the heat and mass transfer model coupled with thermochemical reaction kinetics. The reactor thermal behavior with direct heat transfer between gaseous reactant and products evolution and the effects of different structural parameters were evaluated. It was found that the reactor has the potential to utilize by ～60% of CO_2 captured with 40% of CH_4 co-fed into syngas(72.9% of H_2 and 27.1% of CO) at 741.31 k W/mof incident radiation heat flux. However, the solar irradiance heat flux and temperature distribution were found to significantly affect the reactant species conversion efficiency and syngas production. The chemical reaction is mainly driven by the thermal energy and higher species conversion into syngas was observed when the temperature distribution at the inner cavity of the reactor was more uniform. Designed a solar thermochemical reactor able to volumetric store concentrated irradiance could highly improve CCU technologies for producing energy-rich chemicals. Besides, the mixture gas inlet velocity, operating pressure and CO_2/CH_4 feeding ratio were crucial to determining the efficiency of CO_2 utilization to solar fuels. Catalytic CO_2-reforming of CH_4 to chemical energy is a promising strategy for an efficient utilization of CO_2 as a renewable carbon source.
基金This work was financially supported by the National Key Research and Development Program of China(2018YFA0702002)the Beijing Natural Science Foundation(Z210016)+1 种基金the National Natural Science Foundation of China(51967020,21935001)Shanxi Energy Internet Research Institute(SXEI 2023A004).
文摘The exploration of sustainable energy utilization requires the imple-mentation of advanced electrochemical devices for efficient energy conversion and storage,which are enabled by the usage of cost-effective,high-performance electro-catalysts.Currently,heterogeneous atomically dispersed catalysts are considered as potential candidates for a wide range of applications.Compared to conventional cata-lysts,atomically dispersed metal atoms in carbon-based catalysts have more unsatu-rated coordination sites,quantum size effect,and strong metal-support interactions,resulting in exceptional catalytic activity.Of these,dual-atomic catalysts(DACs)have attracted extensive attention due to the additional synergistic effect between two adja-cent metal atoms.DACs have the advantages of full active site exposure,high selectiv-ity,theoretical 100%atom utilization,and the ability to break the scaling relationship of adsorption free energy on active sites.In this review,we summarize recent research advancement of DACs,which includes(1)the comprehensive understanding of the synergy between atomic pairs;(2)the synthesis of DACs;(3)characterization meth-ods,especially aberration-corrected scanning transmission electron microscopy and synchrotron spectroscopy;and(4)electrochemical energy-related applications.The last part focuses on great potential for the electrochemical catalysis of energy-related small molecules,such as oxygen reduction reaction,CO_(2) reduction reaction,hydrogen evolution reaction,and N_(2) reduction reaction.The future research challenges and opportunities are also raised in prospective section.
文摘Reducing the anthropogenic COemissions from fossil resource combustion and human activities has become one of the major challenges we are facing today.Beyond those practical applications for the utilization of CO,such as the synthesis of salicylic acid,methanol,urea,NaHCO-NaCOchemicals and recently developed polycarbonate synthesis,scientists are still seeking new materials and technologies for efficient capture,
基金supported by National Natural Science Foundation of China (22033009, 22121002, 22238011)。
文摘To improve the electrocatalytic transformation of carbon dioxide (CO_(2)) to multi-carbon (C_(2+)) products is of great importance.Here we developed a nitrogen-doped Cu catalyst,by which the maximum C_(2+) Faradaic efficiency can reach 72.7%in flow-cell system,with the partial current density reaching 0.62 A cm^(-2).The in situ Raman spectra demonstrate that the *CO adsorption can be strengthened on such a N-doped Cu catalyst,thus promoting the *CO utilization in the subsequent C–C coupling step.Simultaneously,the water activation can be well enhanced by N doping on Cu catalyst.Owing to the synergistic effects,the selectivity and activity for C_(2+) products over the N-deoped Cu catalyst are much improved.
