The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both hav...The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both have significant activation barriers, which severely limit the overall performance of energy conversion devices that utilize ORR/OER. Meanwhile, ORR is another very important electrochemical reaction involving oxygen that has been widely investigated. ORR occurs in aqueous solutions via two pathways: the direct 4-electron reduction or 2-electron reduction pathways from O_(2) to water(H_2O) or from O_(2) to hydrogen peroxide(H_2O_(2)). Noble metal electrocatalysts are often used to catalyze OER and ORR, despite the fact that noble metal electrocatalysts have certain intrinsic limitations, such as low storage. Thus, it is urgent to develop more active and stable low-cost electrocatalysts, especially for severe environments(e.g., acidic media). Theoretically, an ideal oxygen electrocatalyst should provide adequate binding to oxygen species. Transition metals not belonging to the platinum group metal-based oxides are a low-cost substance that could give a d orbital for oxygen species binding. As a result, transition metal oxides are regarded as a substitute for typical precious metal oxygen electrocatalysts. However, the development of oxide catalysts for oxygen reduction and oxygen evolution reactions still faces significant challenges, e.g., catalytic activity, stability, cost, and reaction mechanism. We discuss the fundamental principles underlying the design of oxide catalysts, including the influence of crystal structure, and electronic structure on their performance. We also discuss the challenges associated with developing oxide catalysts and the potential strategies to overcome these challenges.展开更多
The investigation of topological transitions has opened up unprecedented avenues for scientific exploration in photonic metamaterials.However,previous studies mainly focused on exploring different types of three-dimen...The investigation of topological transitions has opened up unprecedented avenues for scientific exploration in photonic metamaterials.However,previous studies mainly focused on exploring different types of three-dimensional(3D)equifrequency surfaces and their topological transition processes in magnetic topological systems.In this work,we study the multiple photonic topological transitions and dual-frequency photonic Weyl points in the topological chiral metamaterials.Through effective medium theory and topological band theory,we systematically characterize and draw comprehensive topological phase diagrams associated with diverse 3D equifrequency surface configurations in nonmagnetic photonic systems.We further demonstrate that the resonance frequencyω0 and dual-frequency Weyl points are the critical points of these topological transitions.Notably,when the vacuum state is in contact with the phases I or III chiral metamaterials,the high-local and frequency chirality-dependent topological Fermi arc surface states arise.We reveal that the parameterωcan be used as a degree of freedom to regulate the bandwidth of such topological surface states.Moreover,different types of multichannel and directional topological photonic routings are achieved using the chirality-dependent Fermi arc surface states.We theoretically show that the physical mechanism of achieving these multichannel topological photonic routings is caused by the different interface properties.We could offer promising perspectives on 3D topological semimetal systems and provide more adaptability for multichannel devices in the nonmagnetic continuous media.展开更多
Objective:The previously integrated tumor-inflammation-nutrition(HI-GC)score has demonstrated dynamic monitoring value for recurrence and clinical decision-making in patients with postsurgical gastric cancer(GC).Howev...Objective:The previously integrated tumor-inflammation-nutrition(HI-GC)score has demonstrated dynamic monitoring value for recurrence and clinical decision-making in patients with postsurgical gastric cancer(GC).However,its failure to incorporate clinical-pathological factors limits its capacity for baseline risk assessment.This study aimed to develop a model that accurately identifies patients for adjuvant chemotherapy and dynamically evaluates recurrence risk.Methods:This retrospective,multicenter,longitudinal cohort study,spanning nine hospitals,included 7,085patients with GC post-radical gastrectomy.A baseline prognostic model was constructed using 117 machinelearning algorithms.The dynamic survival decision tree model(dy SDT)was employed to combine the baseline model with the HI-GC score.Results:A Cox regression model incorporating six factors was used to create a nomogram[Harrell's C-index:training cohort:0.765;95%confidence interval(95%CI):0.747,0.783;validation set:0.810;95%CI:0.747,0.783],including p T stage,positive lymph node ratio,p N stage,tumor size,age,and adjuvant chemotherapy.The best-performing machine learning model exhibited similar predictive accuracy to the nomogram(C-index:0.770).For the short-term dy SDT at 1 month,the mortality hazard ratios(HRs)for groups IIa,IIb,andⅢwere 2.61(95%CI:2.24,3.04),5.02(95%CI:4.15,6.06),and 8.88(95%CI:7.57,10.42),respectively,compared to group I.Stratified analysis revealed a significant interaction between adjuvant chemotherapy and overall survival in each subgroup(P<0.001).The long-term dy SDT at 1 year showed HRs of 3.25(95%CI:2.12,4.97)for group II,6.73(95%CI:4.29,10.56)for groupⅢa,and 17.88(95%CI:10.71,29.84)for groupⅢb.Conclusions:The dy SDT effectively stratifies mortality risk and provides valuable assistance in clinical decision-making after gastrectomy.展开更多
In the machining process of aircraft monolithic parts,the initial residual stress redistribution and structural stiffness evolution often lead to unexpected distortions.On the other hand,the stress redistribution and ...In the machining process of aircraft monolithic parts,the initial residual stress redistribution and structural stiffness evolution often lead to unexpected distortions.On the other hand,the stress redistribution and stiffness reduction during the machining process depend on the material removal sequence.The essence of the stress redistribution is releasing the initial elastic strain energy.In the present study,the influence of the material removal sequence on the energy release is studied.Moreover,a novel optimization method is proposed for the material removal sequence.In order to evaluate the performance of the proposed method,the mechanism of the machining distortion is firstly analyzed based on the energy principle.Then a calculative model for the machining distortion of long beam parts is established accordingly.Moreover,an energy parameter related to the bending distortion and the procedure of the material removal sequence optimization is defined.Finally,the bending distortion analysis and material removal sequence optimization are performed on a long beam with a Z-shaped cross-section.Furthermore,simulation and experiments are carried out.The obtained results indicate that the optimized sequence results in a low distortion fluctuation and decreases the bending distortion.展开更多
A cobalt-catalyzed ring-opening/hydroxylation cascade of highly strained cyclopropanols has been developed for the first time. The reaction was conducted under open-air atmosphere to afford a broad series of structura...A cobalt-catalyzed ring-opening/hydroxylation cascade of highly strained cyclopropanols has been developed for the first time. The reaction was conducted under open-air atmosphere to afford a broad series of structurally diverse β-hydroxy ketones in moderate to good yields with high regioselectivity.The protocol features mild reaction conditions, simple operation, high-functional-group tolerance, facile scalability, and heterocycle compatibility.展开更多
Transforming growth factor β plays a role in regulation of apoptosis in CIC-3 and the Smads signaling pathway, although the underlying mechanisms remain unclear. The present study determined possible signal transduct...Transforming growth factor β plays a role in regulation of apoptosis in CIC-3 and the Smads signaling pathway, although the underlying mechanisms remain unclear. The present study determined possible signal transduction mechanisms based on CIC-3 expression, which accordingly affected apoptosis of retinal ganglion cells in a glutamate-induced retinal ganglion cell RGC-5 apoptosis model. Results revealed significantly increased cell survival rate and significantly decreased apoptosis rate following apoptosis of CIC-3 cDNA-transfected glutamate-induced retinal ganglion cells. Following inhibition of the CIC-3 chloride channel using RNAi technology, cell survival and apoptosis rates were reversed. In addition, expression of transforming growth factor β2 Smads2, Smads3, Smads4, and Smads7 increased to varying degrees. These results suggest that CIC-3 chloride channel plays a protective role in glutamate-induced apoptosis of retinal ganglion cells, and transforming growth factor β/Smads signal transduction pathways are involved in this process.展开更多
Over the past few decades,various techniques have been developed for wastewater treatment,among which advanced oxidation processes(AOPs)mediated by transition metal oxide catalysts have received growing attention due ...Over the past few decades,various techniques have been developed for wastewater treatment,among which advanced oxidation processes(AOPs)mediated by transition metal oxide catalysts have received growing attention due to their high efficiency in refractory organic pollutant removal and low toxicity.However,transitionmetal oxides generally induce secondary contaminations by metal leaching and suffer from poor reusability.Herein,guided by computational fluid dynamics(CFD)simulations,a novel hollow fibre reactor fabricated with perovskite-type La_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)(LS CF)was developed to minimize metal leaching and maximize the activation of peroxymonosulfate(PMS)for the removal of ciprofloxacin(CIP,at 20 mg·L^(-1))in wastewater.CIP was wholly degraded after 75 min,and the efficacy of the catalytic process was significantly impacted by both temperature and pH at the onset of the catalytic process.The AOP mechanism was further investigated through electron paramagnetic resonance spectroscopy(EPR),whereby the active species,e.g.,sulfate radicals,singlet oxygen,and hydroxyl,were directly detected.Moreover,the element leaching from the catalytic ceramic hollow-fibre reactor during the aqueous-phase AOP was also investigated through molecular dynamics(MD)simulation and inductively coupled plasma-atomic emission spectroscopy(ICPAES).This catalytic LSCF hollow-fibre reactor demonstrates excellent pollutant degradation with significantly reduced secondary contaminations,which holds promise for further industrial applications.展开更多
The electrochemical conversion of carbon dioxide into valuable products is pivotal for maintaining the global carbon cycle and mitigating global warming.This review explores the advancements in electrochemical CO_(2) ...The electrochemical conversion of carbon dioxide into valuable products is pivotal for maintaining the global carbon cycle and mitigating global warming.This review explores the advancements in electrochemical CO_(2) conversion,particularly focusing on producing methanol,ethanol,and n-propanol using various catalysts such as metals,metal oxides,metal alloys,and metal organic frameworks.Additionally,it covers the photoelectrochemical(PEC)conversion of CO_(2) into alcohols.The primary objective is to identify efficient electrocatalysts for ethanol,methanol,and n-propanol production,prioritizing selectivity,stability,Faradaic efficiency(FE),and current density.Notable catalysts include PtxZn nanoalloys,which exhibit an FE of~81.4% for methanol production,and trimetallic Pt/Pb/Zn nanoalloys,aimed at reducing Pt costs while enhancing catalyst stability and durability.Metal oxide catalysts like thin film Cu_(2)O/CuO on nickel foam and Cu_(2)O/ZnO achieve FE values of~38% and~16.6% for methanol production,respectively.Copper-based metal-organic frameworks,such as Cu@Cu_(2)O,demonstrate an FE of~45% for methanol production.Similarly,Ag_(0.14)/Cu_(0.86) and Cu-Zn alloys exhibit FEs of~63% and~46.6%,respectively,for ethanol production.Notably,n-propanol production via Pd–Cu alloy and graphene/ZnO/Cu_(2)O yields FEs of~13.7% and~23%,respectively.Furthermore,the review discusses recent advancements in PEC reactor design,photoelectrodes,reaction mechanisms,and catalyst durability.By evaluating the efficiency of these devices in liquid fuel production,the review addresses challenges and prospects in CO_(2) conversion for obtaining various valuable products.展开更多
The efficient storage and application of sustainable solar energy has drawn significant attention from both academic and industrial points of view.However,most developed catalytic materials still suffer from insuffici...The efficient storage and application of sustainable solar energy has drawn significant attention from both academic and industrial points of view.However,most developed catalytic materials still suffer from insufficient mass diffusion and unsatisfactory durability due to the lack of interconnected and regulatable porosity.Developing catalytic architectures with engineered active sites and prominent stability through rational synthesis strategies has become one of the core projects in solar-driven applications.The unique properties of mesoporous silicas render them among the most valuable functional materials for industrial applications,such as high specific surface area,regulatable porosity,adjustable surface properties,tunable particle sizes,and great thermal and mechanical stability.Mesoporous silicas serve as structural templates or catalytic supports to enhance light harvesting via the scattering effect and provide large surface areas for active site generation.These advantages have been widely utilized in solar applications,including hydrogen production,CO_(2)conversion,photovoltaics,biomass utilization,and pollutant degradation.To achieve the specific functionalities and desired activity,various types of mesoporous silicas from different synthesis methods have been customized and synthesized.Moreover,morphology regulation and component modification strategies have also been performed to endow mesoporous silica-based materials with unprecedented efficiency for solar energy storage and utilization.Nevertheless,reviews about synthesis,morphology regulation,and component modification strategies for mesoporous silica-based catalyst design in solar-driven applications are still limited.Herein,the latest progress concerning mesoporous silica-based catalysis in solar-driven applications is comprehensively reviewed.Synthesis principles,formation mechanisms,and rational functionalities of mesoporous silica are systematically summarized.Some typical catalysts with impressive activities in different solar-driven applications are highlighted.Furthermore,challenges and future potential opportunities in this study field are also discussed and proposed.This present review guides the design of mesoporous silica catalysts for efficient solar energy management for solar energy storage and conversion applications.展开更多
Nowadays,it is still a challenge to prepared high efficiency and low cost formaldehyde(HCHO)removal catalysts in order to tackle the long-living indoor air pollution.Herein,δ-MnO_(2)is successfully synthesized by a f...Nowadays,it is still a challenge to prepared high efficiency and low cost formaldehyde(HCHO)removal catalysts in order to tackle the long-living indoor air pollution.Herein,δ-MnO_(2)is successfully synthesized by a facile ozonation strategy,where Mn^(2+)is oxidized by ozone(O_(3))bubble in an alkaline solution.It presents one of the best catalytic properties with a low 100%conversion temperature of 85℃for 50 ppm of HCHO under a GHSV of 48,000 mL/(g·hr).As a comparison,more than 6 times far longer oxidation time is needed if O3 is replaced by O_(2).Characterizations show that ozonation process generates a different intermediate of tetragonalβ-HMnO_(2),which would favor the quick transformation into the final productδ-MnO_(2),as compared with the relatively more thermodynamically stable monoclinicγ-HMnO_(2)in the O_(2)process.Finally,HCHO is found to be decomposed into CO_(2)via formate,dioxymethylene and carbonate species as identified by room temperature insitu diffuse reflectance infrared fourier transform spectroscopy.All these results show great potency of this facile ozonation routine for the highly activeδ-MnO_(2)synthesis in order to remove the HCHO contamination.展开更多
Monolithic aerogels are promising candidates for use in atmospheric environmental purification due to their structural advantages,such as fine building block size together with high specific surface area,abundant pore...Monolithic aerogels are promising candidates for use in atmospheric environmental purification due to their structural advantages,such as fine building block size together with high specific surface area,abundant pore structure,etc.Additionally,monolithic aerogels possess a unique monolithic macrostructure that sets them apart from aerogel powders and nanoparticles in practical environmental clean-up applications.This review delves into the available synthesis strategies and atmospheric environmental applications of monolithic aerogels,covering types of monolithic aerogels including SiO_(2),graphene,metal oxides and their combinations,along with their preparation methods.In particular,recent developments for VOC adsorption,CO_(2)capture,catalytic oxidation of VOCs and catalytic reduction of CO_(2)are highlighted.Finally,challenges and future opportunities for monolithic aerogels in the atmospheric environmental purification field are proposed.This reviewprovides valuable insights for designing and utilizing monolithic aerogel-based functional materials.展开更多
基金the Natural Science Foundation of China (22005250)National Key R D Program of China (2022YFB2502000)FWO (12ZV320N)。
文摘The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both have significant activation barriers, which severely limit the overall performance of energy conversion devices that utilize ORR/OER. Meanwhile, ORR is another very important electrochemical reaction involving oxygen that has been widely investigated. ORR occurs in aqueous solutions via two pathways: the direct 4-electron reduction or 2-electron reduction pathways from O_(2) to water(H_2O) or from O_(2) to hydrogen peroxide(H_2O_(2)). Noble metal electrocatalysts are often used to catalyze OER and ORR, despite the fact that noble metal electrocatalysts have certain intrinsic limitations, such as low storage. Thus, it is urgent to develop more active and stable low-cost electrocatalysts, especially for severe environments(e.g., acidic media). Theoretically, an ideal oxygen electrocatalyst should provide adequate binding to oxygen species. Transition metals not belonging to the platinum group metal-based oxides are a low-cost substance that could give a d orbital for oxygen species binding. As a result, transition metal oxides are regarded as a substitute for typical precious metal oxygen electrocatalysts. However, the development of oxide catalysts for oxygen reduction and oxygen evolution reactions still faces significant challenges, e.g., catalytic activity, stability, cost, and reaction mechanism. We discuss the fundamental principles underlying the design of oxide catalysts, including the influence of crystal structure, and electronic structure on their performance. We also discuss the challenges associated with developing oxide catalysts and the potential strategies to overcome these challenges.
基金supported by the Baima Lake Laboratory Joint Fund of the Zhejiang Provincial Natural Science Foundation of China(Grant No.LBMHY25A040002)the National Natural Science Foundation of China(Grant Nos.12304472 and 12304557)+1 种基金the Funds of the Natural Science Foundation of Hangzhou(Grant No.2024SZRYBF050004)the Zhejiang Provincial Natural Science Foundation of China(Grant Nos.ZCLQN25A0401 and ZCLZ25F0502).
文摘The investigation of topological transitions has opened up unprecedented avenues for scientific exploration in photonic metamaterials.However,previous studies mainly focused on exploring different types of three-dimensional(3D)equifrequency surfaces and their topological transition processes in magnetic topological systems.In this work,we study the multiple photonic topological transitions and dual-frequency photonic Weyl points in the topological chiral metamaterials.Through effective medium theory and topological band theory,we systematically characterize and draw comprehensive topological phase diagrams associated with diverse 3D equifrequency surface configurations in nonmagnetic photonic systems.We further demonstrate that the resonance frequencyω0 and dual-frequency Weyl points are the critical points of these topological transitions.Notably,when the vacuum state is in contact with the phases I or III chiral metamaterials,the high-local and frequency chirality-dependent topological Fermi arc surface states arise.We reveal that the parameterωcan be used as a degree of freedom to regulate the bandwidth of such topological surface states.Moreover,different types of multichannel and directional topological photonic routings are achieved using the chirality-dependent Fermi arc surface states.We theoretically show that the physical mechanism of achieving these multichannel topological photonic routings is caused by the different interface properties.We could offer promising perspectives on 3D topological semimetal systems and provide more adaptability for multichannel devices in the nonmagnetic continuous media.
基金supported by the Noncommunicable Chronic Diseases-National Science and Technology Major Project(No.2023ZD0501400)the National Key R&D Program of China(No.2022YFC2505100)the National Natural Science Foundation of China(No.82202837,82421002 and 82350122)。
文摘Objective:The previously integrated tumor-inflammation-nutrition(HI-GC)score has demonstrated dynamic monitoring value for recurrence and clinical decision-making in patients with postsurgical gastric cancer(GC).However,its failure to incorporate clinical-pathological factors limits its capacity for baseline risk assessment.This study aimed to develop a model that accurately identifies patients for adjuvant chemotherapy and dynamically evaluates recurrence risk.Methods:This retrospective,multicenter,longitudinal cohort study,spanning nine hospitals,included 7,085patients with GC post-radical gastrectomy.A baseline prognostic model was constructed using 117 machinelearning algorithms.The dynamic survival decision tree model(dy SDT)was employed to combine the baseline model with the HI-GC score.Results:A Cox regression model incorporating six factors was used to create a nomogram[Harrell's C-index:training cohort:0.765;95%confidence interval(95%CI):0.747,0.783;validation set:0.810;95%CI:0.747,0.783],including p T stage,positive lymph node ratio,p N stage,tumor size,age,and adjuvant chemotherapy.The best-performing machine learning model exhibited similar predictive accuracy to the nomogram(C-index:0.770).For the short-term dy SDT at 1 month,the mortality hazard ratios(HRs)for groups IIa,IIb,andⅢwere 2.61(95%CI:2.24,3.04),5.02(95%CI:4.15,6.06),and 8.88(95%CI:7.57,10.42),respectively,compared to group I.Stratified analysis revealed a significant interaction between adjuvant chemotherapy and overall survival in each subgroup(P<0.001).The long-term dy SDT at 1 year showed HRs of 3.25(95%CI:2.12,4.97)for group II,6.73(95%CI:4.29,10.56)for groupⅢa,and 17.88(95%CI:10.71,29.84)for groupⅢb.Conclusions:The dy SDT effectively stratifies mortality risk and provides valuable assistance in clinical decision-making after gastrectomy.
基金the National Natural Science Foundation of China(No.51405226)。
文摘In the machining process of aircraft monolithic parts,the initial residual stress redistribution and structural stiffness evolution often lead to unexpected distortions.On the other hand,the stress redistribution and stiffness reduction during the machining process depend on the material removal sequence.The essence of the stress redistribution is releasing the initial elastic strain energy.In the present study,the influence of the material removal sequence on the energy release is studied.Moreover,a novel optimization method is proposed for the material removal sequence.In order to evaluate the performance of the proposed method,the mechanism of the machining distortion is firstly analyzed based on the energy principle.Then a calculative model for the machining distortion of long beam parts is established accordingly.Moreover,an energy parameter related to the bending distortion and the procedure of the material removal sequence optimization is defined.Finally,the bending distortion analysis and material removal sequence optimization are performed on a long beam with a Z-shaped cross-section.Furthermore,simulation and experiments are carried out.The obtained results indicate that the optimized sequence results in a low distortion fluctuation and decreases the bending distortion.
基金State Key Basic Research Program of the People's Republic of China(No.2018YFC0310900)National Natural Science Foundation of China(Nos.21871018,21732001)+9 种基金Shenzhen Science and Technology Innovation Committee(Nos.KQTD20190929174023858,JCYJ20180504165454447)Industry and Information Technology Bureau of Shenzhen Municipality(No.201806151622209330)Guangdong Science and Technology Program(No.2017B030314002)Shenzhen-Hong Kong Institute of Brain Science-Shenzhen Fundamental Research Institutions(No.2019SHIBS0004)the National Ten Thousand Talent Program(the Leading Talent Tier)for the financial supportthe Science and Technology Project of Henan Province(No.202102310328)the PhD Start-up Program of Anyang Institute of Technology(No.BSJ 2021042)Guangzhou Basic and Applied Basic Research Project in China(Nos.202102020134,202102020690)Youth Innovation Talents Project of Guangdong Universities(natural science)in China(No.2019KQNCX098)the Henan Postdoctoral Foundation and the Postdoctoral Innovation Base of Anyang Institute of Technology for financial support。
文摘A cobalt-catalyzed ring-opening/hydroxylation cascade of highly strained cyclopropanols has been developed for the first time. The reaction was conducted under open-air atmosphere to afford a broad series of structurally diverse β-hydroxy ketones in moderate to good yields with high regioselectivity.The protocol features mild reaction conditions, simple operation, high-functional-group tolerance, facile scalability, and heterocycle compatibility.
文摘Transforming growth factor β plays a role in regulation of apoptosis in CIC-3 and the Smads signaling pathway, although the underlying mechanisms remain unclear. The present study determined possible signal transduction mechanisms based on CIC-3 expression, which accordingly affected apoptosis of retinal ganglion cells in a glutamate-induced retinal ganglion cell RGC-5 apoptosis model. Results revealed significantly increased cell survival rate and significantly decreased apoptosis rate following apoptosis of CIC-3 cDNA-transfected glutamate-induced retinal ganglion cells. Following inhibition of the CIC-3 chloride channel using RNAi technology, cell survival and apoptosis rates were reversed. In addition, expression of transforming growth factor β2 Smads2, Smads3, Smads4, and Smads7 increased to varying degrees. These results suggest that CIC-3 chloride channel plays a protective role in glutamate-induced apoptosis of retinal ganglion cells, and transforming growth factor β/Smads signal transduction pathways are involved in this process.
基金financially supported by the Key Research and Development Project for the Highlevel Technological Talent of Lvlang city(Nos.2023GXYF09 and 2022RC15)Scientific and Technologial Innovation Programs of Higher Education Institutions in Shanxi(No.2022L558)+2 种基金Scientific Research Start-up Funds of Lyuliang Universitythe support from Royal Society Chemistry(RSC),RSC researcher collaboration grant(No.C23-8220221815)Royce Industrial Collaboration Grant(No.RICP-R4-100029)
文摘Over the past few decades,various techniques have been developed for wastewater treatment,among which advanced oxidation processes(AOPs)mediated by transition metal oxide catalysts have received growing attention due to their high efficiency in refractory organic pollutant removal and low toxicity.However,transitionmetal oxides generally induce secondary contaminations by metal leaching and suffer from poor reusability.Herein,guided by computational fluid dynamics(CFD)simulations,a novel hollow fibre reactor fabricated with perovskite-type La_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)(LS CF)was developed to minimize metal leaching and maximize the activation of peroxymonosulfate(PMS)for the removal of ciprofloxacin(CIP,at 20 mg·L^(-1))in wastewater.CIP was wholly degraded after 75 min,and the efficacy of the catalytic process was significantly impacted by both temperature and pH at the onset of the catalytic process.The AOP mechanism was further investigated through electron paramagnetic resonance spectroscopy(EPR),whereby the active species,e.g.,sulfate radicals,singlet oxygen,and hydroxyl,were directly detected.Moreover,the element leaching from the catalytic ceramic hollow-fibre reactor during the aqueous-phase AOP was also investigated through molecular dynamics(MD)simulation and inductively coupled plasma-atomic emission spectroscopy(ICPAES).This catalytic LSCF hollow-fibre reactor demonstrates excellent pollutant degradation with significantly reduced secondary contaminations,which holds promise for further industrial applications.
基金the financial support from National Science Centre Poland(NCN)based on the decision number UMO-2021/43/D/ST5/00824financial support of research project supported by the program“Excellence Initiative-Research University”for the AGH University of Krakow.
文摘The electrochemical conversion of carbon dioxide into valuable products is pivotal for maintaining the global carbon cycle and mitigating global warming.This review explores the advancements in electrochemical CO_(2) conversion,particularly focusing on producing methanol,ethanol,and n-propanol using various catalysts such as metals,metal oxides,metal alloys,and metal organic frameworks.Additionally,it covers the photoelectrochemical(PEC)conversion of CO_(2) into alcohols.The primary objective is to identify efficient electrocatalysts for ethanol,methanol,and n-propanol production,prioritizing selectivity,stability,Faradaic efficiency(FE),and current density.Notable catalysts include PtxZn nanoalloys,which exhibit an FE of~81.4% for methanol production,and trimetallic Pt/Pb/Zn nanoalloys,aimed at reducing Pt costs while enhancing catalyst stability and durability.Metal oxide catalysts like thin film Cu_(2)O/CuO on nickel foam and Cu_(2)O/ZnO achieve FE values of~38% and~16.6% for methanol production,respectively.Copper-based metal-organic frameworks,such as Cu@Cu_(2)O,demonstrate an FE of~45% for methanol production.Similarly,Ag_(0.14)/Cu_(0.86) and Cu-Zn alloys exhibit FEs of~63% and~46.6%,respectively,for ethanol production.Notably,n-propanol production via Pd–Cu alloy and graphene/ZnO/Cu_(2)O yields FEs of~13.7% and~23%,respectively.Furthermore,the review discusses recent advancements in PEC reactor design,photoelectrodes,reaction mechanisms,and catalyst durability.By evaluating the efficiency of these devices in liquid fuel production,the review addresses challenges and prospects in CO_(2) conversion for obtaining various valuable products.
基金financially supported by the Ningbo Institute of Digital Twin,Eastern Institute of Technology,Ningbo.We also acknowledge supportfrom the Young Innovative Talent of Yongjiang Talent Project(2023A‐387‐G).
文摘The efficient storage and application of sustainable solar energy has drawn significant attention from both academic and industrial points of view.However,most developed catalytic materials still suffer from insufficient mass diffusion and unsatisfactory durability due to the lack of interconnected and regulatable porosity.Developing catalytic architectures with engineered active sites and prominent stability through rational synthesis strategies has become one of the core projects in solar-driven applications.The unique properties of mesoporous silicas render them among the most valuable functional materials for industrial applications,such as high specific surface area,regulatable porosity,adjustable surface properties,tunable particle sizes,and great thermal and mechanical stability.Mesoporous silicas serve as structural templates or catalytic supports to enhance light harvesting via the scattering effect and provide large surface areas for active site generation.These advantages have been widely utilized in solar applications,including hydrogen production,CO_(2)conversion,photovoltaics,biomass utilization,and pollutant degradation.To achieve the specific functionalities and desired activity,various types of mesoporous silicas from different synthesis methods have been customized and synthesized.Moreover,morphology regulation and component modification strategies have also been performed to endow mesoporous silica-based materials with unprecedented efficiency for solar energy storage and utilization.Nevertheless,reviews about synthesis,morphology regulation,and component modification strategies for mesoporous silica-based catalyst design in solar-driven applications are still limited.Herein,the latest progress concerning mesoporous silica-based catalysis in solar-driven applications is comprehensively reviewed.Synthesis principles,formation mechanisms,and rational functionalities of mesoporous silica are systematically summarized.Some typical catalysts with impressive activities in different solar-driven applications are highlighted.Furthermore,challenges and future potential opportunities in this study field are also discussed and proposed.This present review guides the design of mesoporous silica catalysts for efficient solar energy management for solar energy storage and conversion applications.
基金supported by the National Key Research and Development Program of China(No.2016YFC0207100).
文摘Nowadays,it is still a challenge to prepared high efficiency and low cost formaldehyde(HCHO)removal catalysts in order to tackle the long-living indoor air pollution.Herein,δ-MnO_(2)is successfully synthesized by a facile ozonation strategy,where Mn^(2+)is oxidized by ozone(O_(3))bubble in an alkaline solution.It presents one of the best catalytic properties with a low 100%conversion temperature of 85℃for 50 ppm of HCHO under a GHSV of 48,000 mL/(g·hr).As a comparison,more than 6 times far longer oxidation time is needed if O3 is replaced by O_(2).Characterizations show that ozonation process generates a different intermediate of tetragonalβ-HMnO_(2),which would favor the quick transformation into the final productδ-MnO_(2),as compared with the relatively more thermodynamically stable monoclinicγ-HMnO_(2)in the O_(2)process.Finally,HCHO is found to be decomposed into CO_(2)via formate,dioxymethylene and carbonate species as identified by room temperature insitu diffuse reflectance infrared fourier transform spectroscopy.All these results show great potency of this facile ozonation routine for the highly activeδ-MnO_(2)synthesis in order to remove the HCHO contamination.
基金supported by the National Key R&D Program of China(No.2022YFC3702800).
文摘Monolithic aerogels are promising candidates for use in atmospheric environmental purification due to their structural advantages,such as fine building block size together with high specific surface area,abundant pore structure,etc.Additionally,monolithic aerogels possess a unique monolithic macrostructure that sets them apart from aerogel powders and nanoparticles in practical environmental clean-up applications.This review delves into the available synthesis strategies and atmospheric environmental applications of monolithic aerogels,covering types of monolithic aerogels including SiO_(2),graphene,metal oxides and their combinations,along with their preparation methods.In particular,recent developments for VOC adsorption,CO_(2)capture,catalytic oxidation of VOCs and catalytic reduction of CO_(2)are highlighted.Finally,challenges and future opportunities for monolithic aerogels in the atmospheric environmental purification field are proposed.This reviewprovides valuable insights for designing and utilizing monolithic aerogel-based functional materials.
