CO_(2) capture and utilization(CCU)technologies have been recognized as crucial strategies for mitigating global warming,reducing carbon emission,and promoting resource circularity.As such,the design and development o...CO_(2) capture and utilization(CCU)technologies have been recognized as crucial strategies for mitigating global warming,reducing carbon emission,and promoting resource circularity.As such,the design and development of related materials have attracted considerable research attention.Carbon-based materials,characterized by tunable pore structures,abundant active sites,high specific surface area,and excellent chemical stability,demonstrate significant potential for applications in CO_(2) capture and utilization.This review systematically analyzes the adsorption behaviors and performance variations of typical carbon materials,including activated carbon,porous carbon,graphene,and carbon nanotubes during CO_(2) capture processes.Concerning CO_(2) utilization,emphasis is placed on recent advances in the catalytic applications of carbon-based materials in key reactions such as methanation,reverse water-gas shift,dry reforming of methane,and alcohol synthesis.Moreover,the benefits and drawbacks of carbon materials in terms of CO_(2) adsorption capacity,catalytic activity,and stability are thoroughly evaluated,and their potential applications in integrated CO_(2) capture and utilization technologies are discussed.Finally,key strategies for enhancing the performance of carbonaceous materials through structural modulation and surface modification are elucidated.This review aims to provide theoretical guidance for the future development and large-scale implementation of carbon-based materials in CCU technologies.展开更多
Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a no...Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a novel MoS_(2)-Mo_(2)C heterostructure anchored on a carbon sponge(CS)as a Li_(2)S host to solve these problems.A simple hydrothermal process following carbothermal reduction was used to construct the MoS_(2)-Mo_(2)C heterostructure,enabling control of the phases and integration of MoS_(2) and Mo_(2)C.Structural characterization confirmed the coherent interface of the heterostructure with a precise orientation relationship between the two phases and their uniform distribution.An evaluation of the adsorption and catalytic performance of the material showed that it has an exceptional LiPSs adsorption capacity with faster conversion from Li_(2)S_(4) to Li_(2)S_(2).Density functional theory calculations further confirmed these results.As a result,the cathode had a high initial discharge capacity of 693 mAh g^(−1) at 0.2 C and achieved stable cycling at 2 C for 500 cycles with a low decay rate of 0.107%per cycle.The heterostructure design,coupled with the macroporous CS framework,effectively prevented the shuttling and increased sulfur utilization,offering a promising way to produce practical high-energydensity Li–S batteries.展开更多
Photosynthesis of H_(2)O_(2)via sustainable biomass-derived carbon catalysts facilitate the conversion of renewable resources into valuable chemicals.However,the regulatory function of surface functional groups over r...Photosynthesis of H_(2)O_(2)via sustainable biomass-derived carbon catalysts facilitate the conversion of renewable resources into valuable chemicals.However,the regulatory function of surface functional groups over reaction kinetics has not been sufficiently investigated.Herein,hydrothermal carbon spheres(CS)rich in oxygencontaining functional groups demonstrated a remarkably high H_(2)O_(2)production rate(653μmol/(g·h))in both pure water and actual seawater,even in the absence of any sacrificial agent.Meanwhile,the catalyst demonstrates outstanding activity(92%conversion and>99%selectivity)in the visible-light-driven photocatalytic oxidation of benzylamine to imines.Comprehensive analysis reveals that CS was rich in surface oxygen-containing functional groups,a feature strongly associated with its high photocatalytic efficiency.The observed positive Zeta potential of CS in seawater likely diminished the electrostatic repulsion against the positively charged intermediates,thereby facilitating their accumulation at the liquid-solid interface.This work proposes a strategic framework for developing metal-free photocatalysts from biomass,offering a sustainable pathway for photocatalytic applications.展开更多
Porous carbon microspheres are widely regarded as a superior CO_(2) adsorbent due to their exceptional efficiency and affordability.However,better adsorption performance is very attractive for porous carbon microspher...Porous carbon microspheres are widely regarded as a superior CO_(2) adsorbent due to their exceptional efficiency and affordability.However,better adsorption performance is very attractive for porous carbon microspheres.And modification of the pore structure is one of the effective strategies.In this study,multi-cavity mesoporous carbon microspheres were successfully synthesized by the synergistic method of soft and hard templates,during which a phenolic resin with superior thermal stability was employed as the carbon precursor and a mixture of silica sol and F108 as the mesoporous template.Carbon microspheres with multi-cavity mesoporous structures were prepared,and all the samples showed highly even mesopores,with diameters around 12 nm.The diameter of these microspheres decreased from 396.8 nm to about 182.5 nm with the increase of silica sol.After CO_(2) activation,these novel carbon microspheres(APCF0.5-S1.75)demonstrated high specific surface area(983.3 m^(2)/g)and remarkable CO_(2) uptake of 4.93 mmol/g at 0℃ and1 bar.This could be attributed to the unique multi-cavity structure,which offers uniform mesoporous pore channels,minimal CO_(2) transport of and a greater number of active sites for CO_(2) adsorption.展开更多
Dual-carbon batteries(DCBs)have emerged as an appealing candidate for large-scale energy storage,yet the common trade-off between active sites and electronic conduction in carbon materials engenders a main challenge t...Dual-carbon batteries(DCBs)have emerged as an appealing candidate for large-scale energy storage,yet the common trade-off between active sites and electronic conduction in carbon materials engenders a main challenge towards efficient DCBs.Here,we introduce a heteroatom-doped sp^(3) /sp^(2) hybridized carbon fiber membrane(cPAN-Gr)as a universal binder-free active electrode that effectively overcomes this trade-off,enabling efficient Li-ion intercalation chemistry for advanced DCBs.By strategically tuning the sp^(3) and sp^(2) carbon hybridization,the interlayer interaction,geometric and electronic structures of c PANGr are simultaneously optimized,which facilitates rapid Li-ion adsorption,smooth interlayer transport,and efficient electron transport by maximizing the synergy between sp^(2) -and sp^(3) -hybridized carbon.This,coupled with a 3D porous network structure,endows the c PAN-Gr with superior Li-ion storage capability and fast reaction kinetics.Therefore,the c PAN-Gr electrode delivers a high reversible capacity of 345 m A h g^(-1),excellent rate capability(50 C),and an ultralong cycle life over 10,000 cycles,outperforming other reported carbon-based electrodes.Moreover,the constructed DCB exhibits a large specific capacity of 135 m A h g^(-1),long-term cyclability over 500 cycles,and a remarkable energy density of 524.4 Wh kg^(-1).The c PAN-Gr electrode can also be expanded to construct a LiFePO_(4)//cPAN-Gr full battery.Combined theoretical and experimental studies reveal the crucial role of an optimized sp^(3) /sp^(2) ratio(79%)with topological defects and pyridine/pyrrolic N sites on the performance enhancement.This work offers new insights into the design of advanced carbon materials for DCBs and beyond.展开更多
Li_(3)V_(2)(PO_(4))_(3) is a promising high-voltage cathode for zincion batteries,but it suffers from a poor electronic conductivity and vanadium dissolution in aqueous electrolytes.The growth of carboncoated Li_(3)V_...Li_(3)V_(2)(PO_(4))_(3) is a promising high-voltage cathode for zincion batteries,but it suffers from a poor electronic conductivity and vanadium dissolution in aqueous electrolytes.The growth of carboncoated Li_(3)V_(2)(PO_(4))_(3)(LVP@C)nanoparticles on carbon nanofibers(CNFs)has been achieved by an electrospinning technique followed by calcination.The protective carbon coating prevents the aggregation of the LVP nanoparticles and suppresses V dissolution by preventing direct contact with aqueous electrolytes.The CNFs derived from the electrospun nanofibers provide a 3D network to increase the electronic conductivity of the LVP electrode,and the LVP@C-CNF hybrid film can be directly used as a freestanding cathode for zinc-ion batteries without adding conductive additives and binders.A mechanism for the formation of a uniform and continuous carbon coating has been proposed.This nanostructure,combined with the uniform and intact carbon coverage,significantly increases the electronic conductivity.This LVP@C-CNF freestanding electrode has an excellent rate capability(47.3%retention at 2 C)and cycling stability(61.2%retention after 100 cycles)within the voltage range 0.6 V to 1.95 V and is highly suitable for zinc-ion battery applications.展开更多
To promote CO_(2)redox kinetics on the cathode of hybrid sodium-carbon dioxide(Na-CO_(2))batteries,hollow cubic CuS nanoboxes were encapsulated in polypyrrole and polydopamine by in situ polymerization of pyrrole and ...To promote CO_(2)redox kinetics on the cathode of hybrid sodium-carbon dioxide(Na-CO_(2))batteries,hollow cubic CuS nanoboxes were encapsulated in polypyrrole and polydopamine by in situ polymerization of pyrrole and dopamine monomers,respectively,and coupled with high-temperature heat treatment to obtain nitrogen-carbon encapsulated Cu_(x)S@NC_(PPy)and Cu_(x)S@NCPDA catalysts.The results show that the encapsulation of nitrogen-doped carbon not only increases the specific surface area and improves the electron affinity but also promotes the synergistic interaction between the CuS-based active species and the defect carbon,thus providing abundant active sites for CO_(2)conversion.The electrochemical performances of the carbon-coated modified samples were all improved,especially the hybrid Na-CO_(2)battery based on Cu_(x)S@NC_(PPy),which showed a low voltage gap of 0.74 V at 0.1 mA/cm^(2)and a high power density of 3.42 mW/cm^(2).展开更多
Unsecured legacy wells pose significant risks to carbon capture and storage(CCS)as they present potential leakage pathways for stored CO_(2) to return to the atmosphere.In the UK,legacy wells must be assessed for a ca...Unsecured legacy wells pose significant risks to carbon capture and storage(CCS)as they present potential leakage pathways for stored CO_(2) to return to the atmosphere.In the UK,legacy wells must be assessed for a carbon storage permit to be granted and high-risk wells require costly remediation.We use a well risk assessment scheme to evaluate the risk of wells in the Southern North Sea.We then combine our well risk assessment with investigation using the analytical tool CO2BLOCK,which relies on a gravity current model to estimate pressure and plume migration distances.We evaluate the Viking,Camelot and Poseidon projects,which plan to inject CO_(2) into the depleted reservoirs of Southern North Sea gas fields.Carbon dioxide plumes are typically several kilometers wide,and it should be possible to avoid plume migration to high-risk legacy wells.In contrast,pressure fields produced by CO_(2) injection are tens of kilometers wide and low magnitude pressure increases frequently extend beyond the bounds of storage licence areas.The pressure fields encounter hundreds of wells and in the cases of the Camelot and Poseidon projects,interact with each other.展开更多
Ce-TiO2/CA（carbon aerogel） electrode was prepared by sol impregnation approach. The XRD（X-ray diffraction） and Raman spectra reveal that the TiO2 is anatase. The UV-vis diffuse reflectance spectra show that the op...Ce-TiO2/CA（carbon aerogel） electrode was prepared by sol impregnation approach. The XRD（X-ray diffraction） and Raman spectra reveal that the TiO2 is anatase. The UV-vis diffuse reflectance spectra show that the optical absorption edge for Ce-TiO_2/CA is red-shifted to 535 nm compared with TiO_2/CA. Under visible light irradiation, the photocurrent density increment on Ce-TiO_2/CA is 75 times that on Ce-TiO_2/FTO（fluorine-doped tin oxide）. The electrochemical impedance spectroscopy reveals that the conductivity of CeTiO_2/CA is much better than the Ce-TiO_2/FTO. Furthermore, the Ce-TiO_2/CA can be used to the highest electrosorptive photodegradation for 4-chlorophenol wastewater degradation, which is ascribed predominantly to the efficient reduction of electron-hole pair recombination in the photocatalysts.展开更多
基金Supported by National Key R&D Program of China(2025YFE0109700)the National Natural Science Foundation of China(52106150)。
文摘CO_(2) capture and utilization(CCU)technologies have been recognized as crucial strategies for mitigating global warming,reducing carbon emission,and promoting resource circularity.As such,the design and development of related materials have attracted considerable research attention.Carbon-based materials,characterized by tunable pore structures,abundant active sites,high specific surface area,and excellent chemical stability,demonstrate significant potential for applications in CO_(2) capture and utilization.This review systematically analyzes the adsorption behaviors and performance variations of typical carbon materials,including activated carbon,porous carbon,graphene,and carbon nanotubes during CO_(2) capture processes.Concerning CO_(2) utilization,emphasis is placed on recent advances in the catalytic applications of carbon-based materials in key reactions such as methanation,reverse water-gas shift,dry reforming of methane,and alcohol synthesis.Moreover,the benefits and drawbacks of carbon materials in terms of CO_(2) adsorption capacity,catalytic activity,and stability are thoroughly evaluated,and their potential applications in integrated CO_(2) capture and utilization technologies are discussed.Finally,key strategies for enhancing the performance of carbonaceous materials through structural modulation and surface modification are elucidated.This review aims to provide theoretical guidance for the future development and large-scale implementation of carbon-based materials in CCU technologies.
文摘Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a novel MoS_(2)-Mo_(2)C heterostructure anchored on a carbon sponge(CS)as a Li_(2)S host to solve these problems.A simple hydrothermal process following carbothermal reduction was used to construct the MoS_(2)-Mo_(2)C heterostructure,enabling control of the phases and integration of MoS_(2) and Mo_(2)C.Structural characterization confirmed the coherent interface of the heterostructure with a precise orientation relationship between the two phases and their uniform distribution.An evaluation of the adsorption and catalytic performance of the material showed that it has an exceptional LiPSs adsorption capacity with faster conversion from Li_(2)S_(4) to Li_(2)S_(2).Density functional theory calculations further confirmed these results.As a result,the cathode had a high initial discharge capacity of 693 mAh g^(−1) at 0.2 C and achieved stable cycling at 2 C for 500 cycles with a low decay rate of 0.107%per cycle.The heterostructure design,coupled with the macroporous CS framework,effectively prevented the shuttling and increased sulfur utilization,offering a promising way to produce practical high-energydensity Li–S batteries.
基金Supported by the Natural Science Foundation of Shanxi Province(202203021222233,202203021212398,202203021212403)。
文摘Photosynthesis of H_(2)O_(2)via sustainable biomass-derived carbon catalysts facilitate the conversion of renewable resources into valuable chemicals.However,the regulatory function of surface functional groups over reaction kinetics has not been sufficiently investigated.Herein,hydrothermal carbon spheres(CS)rich in oxygencontaining functional groups demonstrated a remarkably high H_(2)O_(2)production rate(653μmol/(g·h))in both pure water and actual seawater,even in the absence of any sacrificial agent.Meanwhile,the catalyst demonstrates outstanding activity(92%conversion and>99%selectivity)in the visible-light-driven photocatalytic oxidation of benzylamine to imines.Comprehensive analysis reveals that CS was rich in surface oxygen-containing functional groups,a feature strongly associated with its high photocatalytic efficiency.The observed positive Zeta potential of CS in seawater likely diminished the electrostatic repulsion against the positively charged intermediates,thereby facilitating their accumulation at the liquid-solid interface.This work proposes a strategic framework for developing metal-free photocatalysts from biomass,offering a sustainable pathway for photocatalytic applications.
基金supported by the National Key R&D Program of China(No.2021YFB3501102).
文摘Porous carbon microspheres are widely regarded as a superior CO_(2) adsorbent due to their exceptional efficiency and affordability.However,better adsorption performance is very attractive for porous carbon microspheres.And modification of the pore structure is one of the effective strategies.In this study,multi-cavity mesoporous carbon microspheres were successfully synthesized by the synergistic method of soft and hard templates,during which a phenolic resin with superior thermal stability was employed as the carbon precursor and a mixture of silica sol and F108 as the mesoporous template.Carbon microspheres with multi-cavity mesoporous structures were prepared,and all the samples showed highly even mesopores,with diameters around 12 nm.The diameter of these microspheres decreased from 396.8 nm to about 182.5 nm with the increase of silica sol.After CO_(2) activation,these novel carbon microspheres(APCF0.5-S1.75)demonstrated high specific surface area(983.3 m^(2)/g)and remarkable CO_(2) uptake of 4.93 mmol/g at 0℃ and1 bar.This could be attributed to the unique multi-cavity structure,which offers uniform mesoporous pore channels,minimal CO_(2) transport of and a greater number of active sites for CO_(2) adsorption.
基金financial support from Guangdong Basic and Applied Basic Research Foundation(2020B1515420001and 2023B1515040027)Fundamental Research Funds for the Central Universities,Sun Yat-sen University(23yxqntd002)the Postdoctoral Fellowship Program of CPSF(GZC20242066)。
文摘Dual-carbon batteries(DCBs)have emerged as an appealing candidate for large-scale energy storage,yet the common trade-off between active sites and electronic conduction in carbon materials engenders a main challenge towards efficient DCBs.Here,we introduce a heteroatom-doped sp^(3) /sp^(2) hybridized carbon fiber membrane(cPAN-Gr)as a universal binder-free active electrode that effectively overcomes this trade-off,enabling efficient Li-ion intercalation chemistry for advanced DCBs.By strategically tuning the sp^(3) and sp^(2) carbon hybridization,the interlayer interaction,geometric and electronic structures of c PANGr are simultaneously optimized,which facilitates rapid Li-ion adsorption,smooth interlayer transport,and efficient electron transport by maximizing the synergy between sp^(2) -and sp^(3) -hybridized carbon.This,coupled with a 3D porous network structure,endows the c PAN-Gr with superior Li-ion storage capability and fast reaction kinetics.Therefore,the c PAN-Gr electrode delivers a high reversible capacity of 345 m A h g^(-1),excellent rate capability(50 C),and an ultralong cycle life over 10,000 cycles,outperforming other reported carbon-based electrodes.Moreover,the constructed DCB exhibits a large specific capacity of 135 m A h g^(-1),long-term cyclability over 500 cycles,and a remarkable energy density of 524.4 Wh kg^(-1).The c PAN-Gr electrode can also be expanded to construct a LiFePO_(4)//cPAN-Gr full battery.Combined theoretical and experimental studies reveal the crucial role of an optimized sp^(3) /sp^(2) ratio(79%)with topological defects and pyridine/pyrrolic N sites on the performance enhancement.This work offers new insights into the design of advanced carbon materials for DCBs and beyond.
文摘Li_(3)V_(2)(PO_(4))_(3) is a promising high-voltage cathode for zincion batteries,but it suffers from a poor electronic conductivity and vanadium dissolution in aqueous electrolytes.The growth of carboncoated Li_(3)V_(2)(PO_(4))_(3)(LVP@C)nanoparticles on carbon nanofibers(CNFs)has been achieved by an electrospinning technique followed by calcination.The protective carbon coating prevents the aggregation of the LVP nanoparticles and suppresses V dissolution by preventing direct contact with aqueous electrolytes.The CNFs derived from the electrospun nanofibers provide a 3D network to increase the electronic conductivity of the LVP electrode,and the LVP@C-CNF hybrid film can be directly used as a freestanding cathode for zinc-ion batteries without adding conductive additives and binders.A mechanism for the formation of a uniform and continuous carbon coating has been proposed.This nanostructure,combined with the uniform and intact carbon coverage,significantly increases the electronic conductivity.This LVP@C-CNF freestanding electrode has an excellent rate capability(47.3%retention at 2 C)and cycling stability(61.2%retention after 100 cycles)within the voltage range 0.6 V to 1.95 V and is highly suitable for zinc-ion battery applications.
基金financially supported by the National Natural Science Foundation of China(No.52172264)the National Key Research and Development Program of China(No.2022YFC3900802)。
文摘To promote CO_(2)redox kinetics on the cathode of hybrid sodium-carbon dioxide(Na-CO_(2))batteries,hollow cubic CuS nanoboxes were encapsulated in polypyrrole and polydopamine by in situ polymerization of pyrrole and dopamine monomers,respectively,and coupled with high-temperature heat treatment to obtain nitrogen-carbon encapsulated Cu_(x)S@NC_(PPy)and Cu_(x)S@NCPDA catalysts.The results show that the encapsulation of nitrogen-doped carbon not only increases the specific surface area and improves the electron affinity but also promotes the synergistic interaction between the CuS-based active species and the defect carbon,thus providing abundant active sites for CO_(2)conversion.The electrochemical performances of the carbon-coated modified samples were all improved,especially the hybrid Na-CO_(2)battery based on Cu_(x)S@NC_(PPy),which showed a low voltage gap of 0.74 V at 0.1 mA/cm^(2)and a high power density of 3.42 mW/cm^(2).
基金supported by the Natural Environment Research Council[grant number NE/S007415/1]Shell as iCASE sponsors。
文摘Unsecured legacy wells pose significant risks to carbon capture and storage(CCS)as they present potential leakage pathways for stored CO_(2) to return to the atmosphere.In the UK,legacy wells must be assessed for a carbon storage permit to be granted and high-risk wells require costly remediation.We use a well risk assessment scheme to evaluate the risk of wells in the Southern North Sea.We then combine our well risk assessment with investigation using the analytical tool CO2BLOCK,which relies on a gravity current model to estimate pressure and plume migration distances.We evaluate the Viking,Camelot and Poseidon projects,which plan to inject CO_(2) into the depleted reservoirs of Southern North Sea gas fields.Carbon dioxide plumes are typically several kilometers wide,and it should be possible to avoid plume migration to high-risk legacy wells.In contrast,pressure fields produced by CO_(2) injection are tens of kilometers wide and low magnitude pressure increases frequently extend beyond the bounds of storage licence areas.The pressure fields encounter hundreds of wells and in the cases of the Camelot and Poseidon projects,interact with each other.
基金Project supported jointly by the Foundation of He'nan Educational Committee(15A150071)
文摘Ce-TiO2/CA（carbon aerogel） electrode was prepared by sol impregnation approach. The XRD（X-ray diffraction） and Raman spectra reveal that the TiO2 is anatase. The UV-vis diffuse reflectance spectra show that the optical absorption edge for Ce-TiO_2/CA is red-shifted to 535 nm compared with TiO_2/CA. Under visible light irradiation, the photocurrent density increment on Ce-TiO_2/CA is 75 times that on Ce-TiO_2/FTO（fluorine-doped tin oxide）. The electrochemical impedance spectroscopy reveals that the conductivity of CeTiO_2/CA is much better than the Ce-TiO_2/FTO. Furthermore, the Ce-TiO_2/CA can be used to the highest electrosorptive photodegradation for 4-chlorophenol wastewater degradation, which is ascribed predominantly to the efficient reduction of electron-hole pair recombination in the photocatalysts.
