A facile and effective impregnation combined with photo-deposition approach was adopted to deposit cadmium sulfide(CdS)nanoparticles on CTF-1,a covalent triazine-based frameworks(CTFs).In this system,CTF-1 not only ac...A facile and effective impregnation combined with photo-deposition approach was adopted to deposit cadmium sulfide(CdS)nanoparticles on CTF-1,a covalent triazine-based frameworks(CTFs).In this system,CTF-1 not only acted as supporter but also served as photocatalyst and electron donor.The performance of the obtained CdS deposited CTF-1(CdS-CTF-1)nanocomposite was evaluated by H2 evolution reaction under visible light irradiation.As a result,CdS-CTF-1 exhibited high H2 production from water,far surpassing the Cd S/CTF-1 nanocomposite,in which Cd S was deposited via solvothermal method.The high activity of CdS-CTF-1 was attributed to the confined Cd S nanoparticles with small size,leading to expose more active sites.In addition,time-resolved spectroscopy indicated that the superior performance of Cd S-CTF-1 also can be ascribed to the fast electron transfer rate and injection efficiency(KET=0.18×10^9 s^-1,ηinj=39.38%)between Cd S and CTF-1 layers,which are 3.83 times faster and 4.84 times higher than that of Cd S/CTF-1 nanocomposite.This work represents the first example on using covalent organic frameworks(COFs)as a support and electron-donor for fabricating novel Cd S-COF nanocomposite system and its potential application in solar energy transformations.展开更多
Herein,we prepa red novel three-dimensional(3D)gear-s haped Co3O4@C(Co3O4 modified by amorphous carbon)and sheet-like SnO2/CC(SnO2 grow on the carbon cloth)as anode and cathode to achieve efficient removal of 4-nitrop...Herein,we prepa red novel three-dimensional(3D)gear-s haped Co3O4@C(Co3O4 modified by amorphous carbon)and sheet-like SnO2/CC(SnO2 grow on the carbon cloth)as anode and cathode to achieve efficient removal of 4-nitrophenol(4-NP)in the presence of peroxymonosulfate(PMS)and simultaneous electrocatalytic reduction of CO2,respectively.In this process,4-NP was mineralized into CO2 by the Co3O4@C,and the generated CO2 was reduced into HCOOH by the sheet-like SnO2/CC cathode.Compared with the pure Co0.5(Co3O4 was prepared using 0.5 g urea)with PMS(30 mg,0.5 g/L),the degradation efficiency of 4-NP(60 mL,10 mg/L)increased from 74.5%-85.1%in 60 min using the Co0.5 modified by amorphous carbon(Co0.5@C).Furthermore,when the voltage of 1.0 V was added in the anodic system of Co0.5@C with PMS(30 mg,0.5 g/L),the degradation efficiency of 4-NP increased from 85.1%-99.1%when Pt was used as cathode.In the experiments of 4-NP degradation coupled with simultaneous electrocatalytic CO2 reduction,the degradation efficiency of 4-NP was 99.0%in the anodic system of Co0.5@C with addition of PMS(30 mg,0.5 g/L),while the Faraday efficiency(FE)of HCOOH was 24.1%at voltage of-1.3 V using the SnO2/CC as cathode.The results showed that the anode of Co3O4 modified by amorphous carbon can markedly improve the degradation efficiency of 4-NP,while the cathode of SnO2/CC can greatly improve the FE and selectivity of CO2 reduction to HCOOH and the stability of cathode.Finally,the promotion mechanism was proposed to explain the degradation of organic pollutants and reduction of CO2 into HCOOH in the process of electrocatalysis coupled with advanced oxidation processes(AOPs)and simultaneous CO2 reduction.展开更多
Rational modification by functional groups was regarded as one of efficient methods to improve the photocatalytic performance of graphitic carbon nitride(g-C3 N4).Herein,g-C3 N4 with yellow(Y-GCN)and brown(C-GCN)were ...Rational modification by functional groups was regarded as one of efficient methods to improve the photocatalytic performance of graphitic carbon nitride(g-C3 N4).Herein,g-C3 N4 with yellow(Y-GCN)and brown(C-GCN)were prepared by using the fresh urea and the urea kept for five years,respectively,for the first time.Experimental results show that the H2 production rate of the C-GCN is 39.06μmol/h,which is about 5 times of the Y-GCN.Meantime,in terms of apparent quantum efficiency(AQ.E)at 420 nm,C-GCN has a value of 6.3%and nearly 7.3 times higher than that of Y-GCN(0.86%).The results of XRD,IR,DRS,and NMR show,different from Y-GCN,a new kind of functional group of—N=CH—was firstly in-situ introduced into the C-GCN,resulting in good visible light absorption,and then markedly improving the photocatalytic performance.DFT calculation also confirms the effect of the—N=CH—group band structure of g-C3N4.Furthermore,XPS results demonstrate that the existence of—N=CH—groups in C-GCN results in tight interaction between C-GCN and Pt nanoparticles,and then improves the charge separation and photocatalytic performance.The present work demonstrates a good example of"defect engineering"to modify the intrinsic molecular structure of g-C3N4 and provides a new avenue to enhance the photocatalytic activity of g-C3N4 via facile and environmental-friendly method.展开更多
Wastewater management and energy/resource recycling have been extensively investigated via photo(electro)catalysis.Although both operation processes are driven effectively by the same interfacial charge,each system is...Wastewater management and energy/resource recycling have been extensively investigated via photo(electro)catalysis.Although both operation processes are driven effectively by the same interfacial charge,each system is practiced separately since they require very different reaction conditions.In this review,we showcase the recent advancements in photo(electro)catalytic process that enables the wastewater treatment and simultaneous energy/resource recovery(WT-ERR).Various literatures based on photo(electro)catalysis for wastewater treatment coupled with CO_(2)conversion,H_(2)production and heavy metal recovery are summarized.Besides,the fundamentals of photo(electro)catalysis and the influencing factors in such synergistic process are also presented.The essential feature of the catalysis lies in effectively utilizing hole oxidation for pollutant degradation and electron reduction for energy/resource recovery.Although in its infancy,the reviewed technology provides new avenue for developing next-generation wastewater treatment process.Moreover,we expect that this review can stimulate intensive researches to rationally design photo(electro)catalytic systems for environmental remediation accompanied with energy and resource recovery.展开更多
Due to the limited permeability and high methane content of the majority of China’s coal seams,significant coal mining gas disasters frequently occur.There is an urgent need to artificially improve the permeability o...Due to the limited permeability and high methane content of the majority of China’s coal seams,significant coal mining gas disasters frequently occur.There is an urgent need to artificially improve the permeability of coalbed methane(CBM)reservoirs,enhance the recovery efficiency of CBM and prevent mine gas accidents.As a novel coal rock fracture technology,the CO_(2) phase transition jet(CPTJ)has been widely used due to its advantages of safety and high fragmentation efficiency.In this study,to ascertain the effects of the pressure of CPTJ fracturing,the influence of its jet pressure on cracked coal rock was revealed,and its effect on CBM extraction was clarified.In this research,the law of CPTJ pressure decay with time was investigated using experimental and theoretical methods.Based on the results,the displacement and discrete fracture network law of CPTJ fracturing coal rock under different jet pressure conditions were studied using particle flow code numerical simulation.Finally,field experiments were conducted at the Shamushu coal mine to assess the efficiency of CPTJ in enhancing CBM drainage.The results showed that the pressure of the CPTJ decreased exponentially with time and significantly influenced the number and expansion size of cracks that broke coal rock but not their direction of development.CPTJ technology can effectively increase the number of connected microscopic pores and fractures in CBM reservoirs,strongly increase the CBM drainage flow rate by between 5.2 and 9.8 times,and significantly reduce the CBM drainage decay coefficient by between 73.58%and 88.24%.展开更多
The development and deployment of giant magnetoimpedance(GMI)sensors have been significantly hampered by their limited sensitivity to weak magnetic fields and pronounced thermal drift phenomena,both of which are intri...The development and deployment of giant magnetoimpedance(GMI)sensors have been significantly hampered by their limited sensitivity to weak magnetic fields and pronounced thermal drift phenomena,both of which are intricately linked to the microstructural properties of the sensor core material,typically composed of metallic glass microwires(MGMWs).Herein,we successfully fabricated an ultra-stable Co-based MGMW with a high GMI effect through a novel multi-step stress-Joule coupled annealing(MS-JCA)technique.The Co-based MGMW showcases a significantly improved GMI effect with an unprecedented impedance change rate of 939%,coupled with an enhanced magnetic field sensitivity of 734%/Oe.In addition,the MS-JCA process ensures the GMI sensor retains exceptional stability during thermal drift measurements over a span of20 h,characterized by a minimal signal fluctuation ratio of merely 0.59%.Notably,the ultra-stability of the GMI sensor arises from the ultra-stable energy state of the MGMWs following MS-JCA.Our findings offer a compelling strategy for significantly enhancing both the performance and stability of GMI sensors,thereby establishing a solid technical foundation for their broader application in weak magnetic detection.展开更多
基金financially supported by the National Natural Science Foundation of China(51938007,51878325,51868050,51622806 and 51868052)the Natural Science Foundation of Jiangxi Province(20162BCB22017,20165BCB18008,20171ACB20017,and 20171BAB206049)+1 种基金the Ph.D.research startup foundation of Nanchang Hangkong University(EA201802367)the foundation of Jiangxi Scientific Committee(DA201902167)for financial support.
文摘A facile and effective impregnation combined with photo-deposition approach was adopted to deposit cadmium sulfide(CdS)nanoparticles on CTF-1,a covalent triazine-based frameworks(CTFs).In this system,CTF-1 not only acted as supporter but also served as photocatalyst and electron donor.The performance of the obtained CdS deposited CTF-1(CdS-CTF-1)nanocomposite was evaluated by H2 evolution reaction under visible light irradiation.As a result,CdS-CTF-1 exhibited high H2 production from water,far surpassing the Cd S/CTF-1 nanocomposite,in which Cd S was deposited via solvothermal method.The high activity of CdS-CTF-1 was attributed to the confined Cd S nanoparticles with small size,leading to expose more active sites.In addition,time-resolved spectroscopy indicated that the superior performance of Cd S-CTF-1 also can be ascribed to the fast electron transfer rate and injection efficiency(KET=0.18×10^9 s^-1,ηinj=39.38%)between Cd S and CTF-1 layers,which are 3.83 times faster and 4.84 times higher than that of Cd S/CTF-1 nanocomposite.This work represents the first example on using covalent organic frameworks(COFs)as a support and electron-donor for fabricating novel Cd S-COF nanocomposite system and its potential application in solar energy transformations.
基金the National Natural Science Foundation of China(Nos.51878325,51868050,51622806,51378246 and 51720105001)the Natural Science Foundation of Jiangxi Province(Nos.20162BCB22017,20165BCB18008,20171ACB20017,20133ACB21001 and 20171BAB206049)the Graduate Innovation Fund of Jiangxi Province(No.YC2018-S360)。
文摘Herein,we prepa red novel three-dimensional(3D)gear-s haped Co3O4@C(Co3O4 modified by amorphous carbon)and sheet-like SnO2/CC(SnO2 grow on the carbon cloth)as anode and cathode to achieve efficient removal of 4-nitrophenol(4-NP)in the presence of peroxymonosulfate(PMS)and simultaneous electrocatalytic reduction of CO2,respectively.In this process,4-NP was mineralized into CO2 by the Co3O4@C,and the generated CO2 was reduced into HCOOH by the sheet-like SnO2/CC cathode.Compared with the pure Co0.5(Co3O4 was prepared using 0.5 g urea)with PMS(30 mg,0.5 g/L),the degradation efficiency of 4-NP(60 mL,10 mg/L)increased from 74.5%-85.1%in 60 min using the Co0.5 modified by amorphous carbon(Co0.5@C).Furthermore,when the voltage of 1.0 V was added in the anodic system of Co0.5@C with PMS(30 mg,0.5 g/L),the degradation efficiency of 4-NP increased from 85.1%-99.1%when Pt was used as cathode.In the experiments of 4-NP degradation coupled with simultaneous electrocatalytic CO2 reduction,the degradation efficiency of 4-NP was 99.0%in the anodic system of Co0.5@C with addition of PMS(30 mg,0.5 g/L),while the Faraday efficiency(FE)of HCOOH was 24.1%at voltage of-1.3 V using the SnO2/CC as cathode.The results showed that the anode of Co3O4 modified by amorphous carbon can markedly improve the degradation efficiency of 4-NP,while the cathode of SnO2/CC can greatly improve the FE and selectivity of CO2 reduction to HCOOH and the stability of cathode.Finally,the promotion mechanism was proposed to explain the degradation of organic pollutants and reduction of CO2 into HCOOH in the process of electrocatalysis coupled with advanced oxidation processes(AOPs)and simultaneous CO2 reduction.
基金financial support of the National Natural Science Foundation of China(NSFC,Nos.51622806,51878325,51868050,51378246 and 51720105001)the Natural Science Foundation of Jiangxi Province(Nos.20162BCB22017,20165BCB18008,20171ACB20017,20133ACB21001 and 20171BAB206049)。
文摘Rational modification by functional groups was regarded as one of efficient methods to improve the photocatalytic performance of graphitic carbon nitride(g-C3 N4).Herein,g-C3 N4 with yellow(Y-GCN)and brown(C-GCN)were prepared by using the fresh urea and the urea kept for five years,respectively,for the first time.Experimental results show that the H2 production rate of the C-GCN is 39.06μmol/h,which is about 5 times of the Y-GCN.Meantime,in terms of apparent quantum efficiency(AQ.E)at 420 nm,C-GCN has a value of 6.3%and nearly 7.3 times higher than that of Y-GCN(0.86%).The results of XRD,IR,DRS,and NMR show,different from Y-GCN,a new kind of functional group of—N=CH—was firstly in-situ introduced into the C-GCN,resulting in good visible light absorption,and then markedly improving the photocatalytic performance.DFT calculation also confirms the effect of the—N=CH—group band structure of g-C3N4.Furthermore,XPS results demonstrate that the existence of—N=CH—groups in C-GCN results in tight interaction between C-GCN and Pt nanoparticles,and then improves the charge separation and photocatalytic performance.The present work demonstrates a good example of"defect engineering"to modify the intrinsic molecular structure of g-C3N4 and provides a new avenue to enhance the photocatalytic activity of g-C3N4 via facile and environmental-friendly method.
基金financially supported by the National Natural Science Foundation of China(Nos.52000097,51878325,51868050 and 51938007)the Natural Science Foundation of Jiangxi Province(Nos.20192BAB213011 and 20192ACBL21046)+1 种基金the Ph.D.research startup foundation of Nanchang Hangkong University(No.EA201802367)the Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment(No.SKLPEE-KF202106),Fuzhou University。
文摘Wastewater management and energy/resource recycling have been extensively investigated via photo(electro)catalysis.Although both operation processes are driven effectively by the same interfacial charge,each system is practiced separately since they require very different reaction conditions.In this review,we showcase the recent advancements in photo(electro)catalytic process that enables the wastewater treatment and simultaneous energy/resource recovery(WT-ERR).Various literatures based on photo(electro)catalysis for wastewater treatment coupled with CO_(2)conversion,H_(2)production and heavy metal recovery are summarized.Besides,the fundamentals of photo(electro)catalysis and the influencing factors in such synergistic process are also presented.The essential feature of the catalysis lies in effectively utilizing hole oxidation for pollutant degradation and electron reduction for energy/resource recovery.Although in its infancy,the reviewed technology provides new avenue for developing next-generation wastewater treatment process.Moreover,we expect that this review can stimulate intensive researches to rationally design photo(electro)catalytic systems for environmental remediation accompanied with energy and resource recovery.
基金the National Natural Science Foundation of China(Grant Nos.52204095,51974163,52274127 and 52174174)the National Key Research and Development Program of China(No.2021YFC2902104)+3 种基金the Natural Science Foundation of Hunan Province,China(No.2023JJ30509)the Key Laboratory of Safety and High-efficiency Coal Mining of Ministry of Education(No.JYBSYS2020204)the Special Program for Basic Research of Key Scientific Research Projects of Colleges and Universities in Henan Province of China(No.21ZX004)the Innovative Scientific Research Team of Henan Polytechnic University in China(No.T2022-1).
文摘Due to the limited permeability and high methane content of the majority of China’s coal seams,significant coal mining gas disasters frequently occur.There is an urgent need to artificially improve the permeability of coalbed methane(CBM)reservoirs,enhance the recovery efficiency of CBM and prevent mine gas accidents.As a novel coal rock fracture technology,the CO_(2) phase transition jet(CPTJ)has been widely used due to its advantages of safety and high fragmentation efficiency.In this study,to ascertain the effects of the pressure of CPTJ fracturing,the influence of its jet pressure on cracked coal rock was revealed,and its effect on CBM extraction was clarified.In this research,the law of CPTJ pressure decay with time was investigated using experimental and theoretical methods.Based on the results,the displacement and discrete fracture network law of CPTJ fracturing coal rock under different jet pressure conditions were studied using particle flow code numerical simulation.Finally,field experiments were conducted at the Shamushu coal mine to assess the efficiency of CPTJ in enhancing CBM drainage.The results showed that the pressure of the CPTJ decreased exponentially with time and significantly influenced the number and expansion size of cracks that broke coal rock but not their direction of development.CPTJ technology can effectively increase the number of connected microscopic pores and fractures in CBM reservoirs,strongly increase the CBM drainage flow rate by between 5.2 and 9.8 times,and significantly reduce the CBM drainage decay coefficient by between 73.58%and 88.24%.
基金supported by the National Natural Science Foundation of China(Grant Nos.52192602,62488201,52071222,51925103,5227114952201183)+7 种基金the Guangdong Major Project of Basic and Applied Basic Research,China(Grant No.2019B030302010)the Guangdong Basic and Applied Basic Research Foundation(Grant No.2023A1515110145)the National Key Research and Development Program of China(Grant No.2021YFA0716302)the Innovation Program of Shanghai Municipal Education Commission(Grant No.2021-01-07-00-09-E00114)the Innovation Program of Shanghai Science and Technology(Grant No.23520760700)the Aviation Foundation(Grant No.2023Z0530S6004)the financial support from Program 173(Grant No.2020-JCIQ-ZD-186-01)the Space Utilization System of China Manned Space Engineering(Grant No.KJZ-YY-NCL08)。
文摘The development and deployment of giant magnetoimpedance(GMI)sensors have been significantly hampered by their limited sensitivity to weak magnetic fields and pronounced thermal drift phenomena,both of which are intricately linked to the microstructural properties of the sensor core material,typically composed of metallic glass microwires(MGMWs).Herein,we successfully fabricated an ultra-stable Co-based MGMW with a high GMI effect through a novel multi-step stress-Joule coupled annealing(MS-JCA)technique.The Co-based MGMW showcases a significantly improved GMI effect with an unprecedented impedance change rate of 939%,coupled with an enhanced magnetic field sensitivity of 734%/Oe.In addition,the MS-JCA process ensures the GMI sensor retains exceptional stability during thermal drift measurements over a span of20 h,characterized by a minimal signal fluctuation ratio of merely 0.59%.Notably,the ultra-stability of the GMI sensor arises from the ultra-stable energy state of the MGMWs following MS-JCA.Our findings offer a compelling strategy for significantly enhancing both the performance and stability of GMI sensors,thereby establishing a solid technical foundation for their broader application in weak magnetic detection.
