Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology r...Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.展开更多
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
The new-generation electronic components require a balance between electromagnetic interference shielding efficiency and open structure factors such as ventilation and heat dissipation.In addition,realizing the tunabl...The new-generation electronic components require a balance between electromagnetic interference shielding efficiency and open structure factors such as ventilation and heat dissipation.In addition,realizing the tunable shielding of porous shields over a wide range of wavelengths is even more challenging.In this study,the well-prepared thermoplastic polyurethane/carbon nanotubes composites were used to fabricate the novel periodic porous flexible metamaterials using fused deposition modeling 3D printing.Particularly,the investigation focuses on optimization of pore geometry,size,dislocation configuration and material thickness,thus establishing a clear correlation between structural parameters and shielding property.Both experimental and simulation results have validated the superior shielding performance of hexagon derived honeycomb structure over other designs,and proposed the failure shielding size(D_(f)≈λ/8-λ/5)and critical inclined angle(θf≈43°-48°),which could be used as new benchmarks for tunable electromagnetic shielding.In addition,the proper regulation of the material thickness could remarkably enhance the maximum shielding capability(85-95 dB)and absorption coefficient A(over 0.83).The final innovative design of the porous shielding box also exhibits good shielding effectiveness across a broad frequency range(over 2.4 GHz),opening up novel pathways for individualized and diversified shielding solutions.展开更多
基金financially supported by the National Natural Science Foundation of China (Nos.U2002212,52102058,52204414,52204413,and 52204412)the National Key R&D Program of China (Nos.2021YFC1910504,2019YFC1907101,2019YFC1907103,and 2017YFB0702304)+7 种基金the Key R&D Program of Ningxia Hui Autonomous Region,China (Nos.2021BEG01003 and2020BCE01001)the Xijiang Innovation and Entrepreneurship Team,China (No.2017A0109004)the Macao Young Scholars Program (No.AM2022024),Chinathe Beijing Natural Science Foundation (Nos.L212020 and 2214073),Chinathe Guangdong Basic and Applied Basic Research Foundation,China (Nos.2021A1515110998 and 2020A1515110408)the China Postdoctoral Science Foundation (No.2022M710349)the Fundamental Research Funds for the Central Universities,China (Nos.FRF-BD-20-24A,FRF-TP-20-031A1,FRF-IC-19-017Z,and 06500141)the Integration of Green Key Process Systems MIIT and Scientific and Technological Innovation Foundation of Foshan,China(Nos.BK22BE001 and BK21BE002)。
文摘Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.
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supported by the National Key R&D Program of China(2023YFB4603504)the International Science&Technology Innovation Cooperation Project of Sichuan Province(2024YFHZ0232)+2 种基金the International Science&Technology Cooperation Project of Chengdu(2021-GH03-00009-HZ)the Program for Featured Directions of Engineering Multi-disciplines of Sichuan University(2020SCUNG203)the Program of Innovative Research Team for Young Scientists of Sichuan Province(22CXTD0019).
文摘The new-generation electronic components require a balance between electromagnetic interference shielding efficiency and open structure factors such as ventilation and heat dissipation.In addition,realizing the tunable shielding of porous shields over a wide range of wavelengths is even more challenging.In this study,the well-prepared thermoplastic polyurethane/carbon nanotubes composites were used to fabricate the novel periodic porous flexible metamaterials using fused deposition modeling 3D printing.Particularly,the investigation focuses on optimization of pore geometry,size,dislocation configuration and material thickness,thus establishing a clear correlation between structural parameters and shielding property.Both experimental and simulation results have validated the superior shielding performance of hexagon derived honeycomb structure over other designs,and proposed the failure shielding size(D_(f)≈λ/8-λ/5)and critical inclined angle(θf≈43°-48°),which could be used as new benchmarks for tunable electromagnetic shielding.In addition,the proper regulation of the material thickness could remarkably enhance the maximum shielding capability(85-95 dB)and absorption coefficient A(over 0.83).The final innovative design of the porous shielding box also exhibits good shielding effectiveness across a broad frequency range(over 2.4 GHz),opening up novel pathways for individualized and diversified shielding solutions.