Mineral carbonation is a promising CO_(2) sequestration strategy that can utilize industrial wastes to convert CO_(2) into high-value CaCO_(3).This review summarizes the advancements in CO_(2) mineralization using typ...Mineral carbonation is a promising CO_(2) sequestration strategy that can utilize industrial wastes to convert CO_(2) into high-value CaCO_(3).This review summarizes the advancements in CO_(2) mineralization using typical industrial wastes to prepare ultrafine CaCO_(3).This work surveys the mechanisms of CO_(2) mineralization using these wastes and its capacities to synthesize CaCO_(3),evaluates the effects of carbonation pathways and operating parameters on the preparation of CaCO_(3),analyzes the current industrial application status and economics of this technology.Due to the large amount of impurities in solid wastes,the purity of CaCO_(3) prepared by indirect methods is greater than that prepared by direct methods.Crystalline CaCO_(3) includes three polymorphs.The polymorph of CaCO_(3) synthesized by carbonation process is determined the combined effects of various factors.These parameters essentially impact the nucleation and growth of CaCO_(3) by altering the CO_(2) supersaturation in the reaction system and the surface energy of CaCO_(3) grains.Increasing the initial pH of the solution and the CO_(2)flow rate favors the formation of vaterite,but calcite is formed under excessively high pH.Vaterite formation is favored at lower temperatures and residence time.With increased temperature and prolonged residence time,it passes through aragonite metastable phase and eventually transforms into calcite.Moreover,polymorph modifiers can decrease the surface energy of CaCO_(3) grains,facilitating the synthesis of vaterite.However,the large-scale application of this technology still faces many problems,including high costs,high energy consumption,low calcium leaching rate,low carbonation efficiency,and low product yield.Therefore,it is necessary to investigate ways to accelerate carbonation,optimize operating parameters,develop cost-effective agents,and understand the kinetics of CaCO_(3) nucleation and crystallization to obtain products with specific crystal forms.Furthermore,more studies on life cycle assessment(LCA)should be conducted to fully confirm the feasibility of the developed technologies.展开更多
Considering their superior theoretical capacity and low voltage plateau,bismuth(Bi)-based materials are being widely explored for application in potassium-ion batteries(PIBs).Unfortunately,pure Bi and Bibased compound...Considering their superior theoretical capacity and low voltage plateau,bismuth(Bi)-based materials are being widely explored for application in potassium-ion batteries(PIBs).Unfortunately,pure Bi and Bibased compounds suffer from severe electrochemical polarization,agglomeration,and dramatic volume fluctuations.To develop an advanced bismuth-based anode material with high reactivity and durability,in this work,the pyrolysis of Bi-based metal-organic frameworks and in-situ selenization techniques have been successfully used to produce a Bi-based composite with high capacity and unique structure,in which Bi/Bi_(3)Se_(4)nanoparticles are encapsulated in carbon nanorods(Bi/Bi_(3)Se_(4)@CNR).Applied as the anode material of PIBs,the Bi/Bi_(3)Se_(4)@CNR displays fast potassium storage capability with 307.5 m A h g^(-1)at 20 A g^(-1)and durable cycle performance of 2000 cycles at 5 A g^(-1).Notably,the Bi/Bi_(3)Se_(4)@CNR also showed long cycle stability over 1600 cycles when working in a full cell system with potassium vanadate as the cathode material,which further demonstrates its promising potential in the field of PIBs.Additionally,the dual potassium storage mechanism of the Bi/Bi_(3)Se_(4)@CNR based on conversion and alloying reaction has also been revealed by in-situ X-ray diffraction.展开更多
In the carbonate industry,deep decarbonization strategies are necessary to effectively remediate CO_(2).These strategies mainly include both sustainable energy supplies and the conversion of CO_(2)in downstream proces...In the carbonate industry,deep decarbonization strategies are necessary to effectively remediate CO_(2).These strategies mainly include both sustainable energy supplies and the conversion of CO_(2)in downstream processes.This study developed a coupled process of biomass chemical looping H2 production and reductive calcination of CaCO_(3).Firstly,a mass and energy balance of the coupled process was established in Aspen Plus.Following this,process optimization and energy integration were implemented to provide optimized operation conditions.Lastly,a life cycle assessment was carried out to assess the carbon footprint of the coupled process.Results reveal that the decomposition temperature of CaCO_(3)in an H_(2)atmosphere can be reduced to 780℃(generally around 900℃),and the conversion of CO_(2)from CaCO_(3)decomposition reached 81.33%with an H2:CO ratio of 2.49 in gaseous products.By optimizing systemic energy through heat integration,an energy efficiency of 86.30%was achieved.Additionally,the carbon footprint analysis revealed that the process with energy integration had a low global warming potential(GWP)of-2.624 kg·kg^(-1)(CO_(2)/CaO).Conclusively,this work performed a systematic analysis of introducing biomass-derived H_(2)into CaCO_(3)calcination and demonstrated the positive role of reductive calcination using green H_(2)in mitigating CO_(2)emissions within the carbonate industry.展开更多
For decades,distiller waste and CO_(2) were not the first choice for production of high valued products.Here,CaCO_(3) hollow microspheres,a high-value product was synthesized from such a reaction system.The synthetic ...For decades,distiller waste and CO_(2) were not the first choice for production of high valued products.Here,CaCO_(3) hollow microspheres,a high-value product was synthesized from such a reaction system.The synthetic methods,the formation mechanism and operational cost were discussed.When 2.5 L·min^(–1)·L^(–1) CO_(2) was flowed into distiller waste(pH=11.4),spheres with 4–13μm diameters and about 2μm shell thickness were obtained.It is found that there is a transformation of CaCO_(3) particles from solid-cubic nuclei to hollow spheres.Firstly,the Ca(OH)_(2) in the distiller waste stimulated the nucleation of calcite with a non-template effect and further maintained the calcite form and prevented the formation of vaterite.Therefore,in absence of auxiliaries,the formation of hollow structures mainly depended on the growth and aging of CaCO_(3).Studies on the crystal morphology and its changes during the growth process point to the inside–out Ostwald effect in the formation of hollow spheres.Change in chemical properties of the bulk solution caused changes in interfacial tension and interfacial energy,which promoted the morphological transformation of CaCO_(3) particles from cubic calcite to spherical clusters.Finally,the flow process for absorption of CO_(2) by distiller waste was designed and found profitable.展开更多
Great efforts have been devoted to improve the photocatalytic activity of TiO2 in the visible light region. Rational design of the external structure and adjustment of intrinsic electronic status by impurity doping ar...Great efforts have been devoted to improve the photocatalytic activity of TiO2 in the visible light region. Rational design of the external structure and adjustment of intrinsic electronic status by impurity doping are two main effective ways to achieve this purpose. A facile onepot synthetic approach was developed to prepare C-doped hollow TiO2 spheres, which simultaneously realized these advantages. The synthesized TiO2 exhibits a mesoporous hollow spherical structure composed of fine nanocrystals, leading to high specific surface area(~180 m^2/g) and versatile porous texture. Carbonate-doping was achieved by a postthermal treatment at a relatively low temperature(200°C), which makes the absorption edge red-shifted to the visible region of the solar spectrum. Concomitantly, Ti^(3+) induced by C-doping also functions in improving the visible-light photocatalytic activity by reducing the band gap. There exists a synergistic effect from multiple stimulatives to enhance the photocatalytic effect of the prepared TiO2 catalyst. It is not out of expectation that the asprepared C-doped hollow TiO2 spheres exhibits an improved photocatalytic activity under visible light irradiation in organic pollutant degradation.展开更多
基金support was received the Science&Technology Foundation of RIPP(PR20230092,PR20230259)the National Natural Science Foundation of China(22278419)the Key Core Technology Research(Social Development)Foundation of Suzhou(2023ss06).
文摘Mineral carbonation is a promising CO_(2) sequestration strategy that can utilize industrial wastes to convert CO_(2) into high-value CaCO_(3).This review summarizes the advancements in CO_(2) mineralization using typical industrial wastes to prepare ultrafine CaCO_(3).This work surveys the mechanisms of CO_(2) mineralization using these wastes and its capacities to synthesize CaCO_(3),evaluates the effects of carbonation pathways and operating parameters on the preparation of CaCO_(3),analyzes the current industrial application status and economics of this technology.Due to the large amount of impurities in solid wastes,the purity of CaCO_(3) prepared by indirect methods is greater than that prepared by direct methods.Crystalline CaCO_(3) includes three polymorphs.The polymorph of CaCO_(3) synthesized by carbonation process is determined the combined effects of various factors.These parameters essentially impact the nucleation and growth of CaCO_(3) by altering the CO_(2) supersaturation in the reaction system and the surface energy of CaCO_(3) grains.Increasing the initial pH of the solution and the CO_(2)flow rate favors the formation of vaterite,but calcite is formed under excessively high pH.Vaterite formation is favored at lower temperatures and residence time.With increased temperature and prolonged residence time,it passes through aragonite metastable phase and eventually transforms into calcite.Moreover,polymorph modifiers can decrease the surface energy of CaCO_(3) grains,facilitating the synthesis of vaterite.However,the large-scale application of this technology still faces many problems,including high costs,high energy consumption,low calcium leaching rate,low carbonation efficiency,and low product yield.Therefore,it is necessary to investigate ways to accelerate carbonation,optimize operating parameters,develop cost-effective agents,and understand the kinetics of CaCO_(3) nucleation and crystallization to obtain products with specific crystal forms.Furthermore,more studies on life cycle assessment(LCA)should be conducted to fully confirm the feasibility of the developed technologies.
基金financially supported by the National Natural Science Foundation of China (22209057)the Guangdong Basic and Applied Basic Research Foundation (2021A1515010362)+1 种基金the Guangzhou Basic and Applied Basic Research Foundation (202102020995)the Open Fund of Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications (2020B121201005)。
文摘Considering their superior theoretical capacity and low voltage plateau,bismuth(Bi)-based materials are being widely explored for application in potassium-ion batteries(PIBs).Unfortunately,pure Bi and Bibased compounds suffer from severe electrochemical polarization,agglomeration,and dramatic volume fluctuations.To develop an advanced bismuth-based anode material with high reactivity and durability,in this work,the pyrolysis of Bi-based metal-organic frameworks and in-situ selenization techniques have been successfully used to produce a Bi-based composite with high capacity and unique structure,in which Bi/Bi_(3)Se_(4)nanoparticles are encapsulated in carbon nanorods(Bi/Bi_(3)Se_(4)@CNR).Applied as the anode material of PIBs,the Bi/Bi_(3)Se_(4)@CNR displays fast potassium storage capability with 307.5 m A h g^(-1)at 20 A g^(-1)and durable cycle performance of 2000 cycles at 5 A g^(-1).Notably,the Bi/Bi_(3)Se_(4)@CNR also showed long cycle stability over 1600 cycles when working in a full cell system with potassium vanadate as the cathode material,which further demonstrates its promising potential in the field of PIBs.Additionally,the dual potassium storage mechanism of the Bi/Bi_(3)Se_(4)@CNR based on conversion and alloying reaction has also been revealed by in-situ X-ray diffraction.
基金support from the National Natural Science Foundation of China(21978128,91934302)partial support from the State Key Laboratory of Materials-oriented Chemical Engineering(ZK202006)also acknowledged.Additionallysupported by the“Cultivation Program for The Excellent Doctoral Dissertation of Nanjing Tech University(3800124701)”.
文摘In the carbonate industry,deep decarbonization strategies are necessary to effectively remediate CO_(2).These strategies mainly include both sustainable energy supplies and the conversion of CO_(2)in downstream processes.This study developed a coupled process of biomass chemical looping H2 production and reductive calcination of CaCO_(3).Firstly,a mass and energy balance of the coupled process was established in Aspen Plus.Following this,process optimization and energy integration were implemented to provide optimized operation conditions.Lastly,a life cycle assessment was carried out to assess the carbon footprint of the coupled process.Results reveal that the decomposition temperature of CaCO_(3)in an H_(2)atmosphere can be reduced to 780℃(generally around 900℃),and the conversion of CO_(2)from CaCO_(3)decomposition reached 81.33%with an H2:CO ratio of 2.49 in gaseous products.By optimizing systemic energy through heat integration,an energy efficiency of 86.30%was achieved.Additionally,the carbon footprint analysis revealed that the process with energy integration had a low global warming potential(GWP)of-2.624 kg·kg^(-1)(CO_(2)/CaO).Conclusively,this work performed a systematic analysis of introducing biomass-derived H_(2)into CaCO_(3)calcination and demonstrated the positive role of reductive calcination using green H_(2)in mitigating CO_(2)emissions within the carbonate industry.
基金This work is supported by the National Natural Science Foundation of China(Grant Nos.U20A20149,21878180 and 21908137)the Graduate Education Project of Shanxi Province(NO.2021Y139).
文摘For decades,distiller waste and CO_(2) were not the first choice for production of high valued products.Here,CaCO_(3) hollow microspheres,a high-value product was synthesized from such a reaction system.The synthetic methods,the formation mechanism and operational cost were discussed.When 2.5 L·min^(–1)·L^(–1) CO_(2) was flowed into distiller waste(pH=11.4),spheres with 4–13μm diameters and about 2μm shell thickness were obtained.It is found that there is a transformation of CaCO_(3) particles from solid-cubic nuclei to hollow spheres.Firstly,the Ca(OH)_(2) in the distiller waste stimulated the nucleation of calcite with a non-template effect and further maintained the calcite form and prevented the formation of vaterite.Therefore,in absence of auxiliaries,the formation of hollow structures mainly depended on the growth and aging of CaCO_(3).Studies on the crystal morphology and its changes during the growth process point to the inside–out Ostwald effect in the formation of hollow spheres.Change in chemical properties of the bulk solution caused changes in interfacial tension and interfacial energy,which promoted the morphological transformation of CaCO_(3) particles from cubic calcite to spherical clusters.Finally,the flow process for absorption of CO_(2) by distiller waste was designed and found profitable.
基金supported by the National Natural Science Foundation of China(Nos.21677159,21522706,21677167)the National Basic Research Program of China(2011CB936001)the Thousand Young Talents Program of China
文摘Great efforts have been devoted to improve the photocatalytic activity of TiO2 in the visible light region. Rational design of the external structure and adjustment of intrinsic electronic status by impurity doping are two main effective ways to achieve this purpose. A facile onepot synthetic approach was developed to prepare C-doped hollow TiO2 spheres, which simultaneously realized these advantages. The synthesized TiO2 exhibits a mesoporous hollow spherical structure composed of fine nanocrystals, leading to high specific surface area(~180 m^2/g) and versatile porous texture. Carbonate-doping was achieved by a postthermal treatment at a relatively low temperature(200°C), which makes the absorption edge red-shifted to the visible region of the solar spectrum. Concomitantly, Ti^(3+) induced by C-doping also functions in improving the visible-light photocatalytic activity by reducing the band gap. There exists a synergistic effect from multiple stimulatives to enhance the photocatalytic effect of the prepared TiO2 catalyst. It is not out of expectation that the asprepared C-doped hollow TiO2 spheres exhibits an improved photocatalytic activity under visible light irradiation in organic pollutant degradation.