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Self-assembled S-scheme In_(2.77)S_(4)/K^(+)-doped g-C_(3)N_(4)photocatalyst with selective O_(2)reduction pathway for efficient H_(2)O_(2)production using water and air
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作者 Qiqi Zhang Hui Miao +2 位作者 Jun Wang Tao Sun Enzhou Liu 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第8期176-189,共14页
The development of an efficient artificial H_(2)O_(2)photosynthesis system is a challenging work using H_(2)O and O_(2)as starting materials.Herein,3D In2.77S_(4)nanoflower precursor was in-situ deposited on K^(+)-dop... The development of an efficient artificial H_(2)O_(2)photosynthesis system is a challenging work using H_(2)O and O_(2)as starting materials.Herein,3D In2.77S_(4)nanoflower precursor was in-situ deposited on K^(+)-doped g-C_(3)N_(4)(KCN)nanosheets using a solvothermal method,then In2.77S_(4)/KCN(IS/KCN)het-erojunction with an intimate interface was obtained after a calcination process.The investigation shows that the photocatalytic H_(2)O_(2)production rate of 50IS/KCN can reach up to 1.36 mmol g^(-1)h^(-1)without any sacrificial reagents under visible light irradiation,which is 9.2 times and 4.1 times higher than that of KCN and In2.77S_(4),respectively.The enhanced activity of the above composite can be mainly attributed to the S-scheme charge transfer route between KCN and In2.77S_(4)according to density functional theory calculations,electron paramagnetic resonance and free radical capture tests,leading to an expanded light response range and rapid charge separation at their interface,as well as preserving the active electrons and holes for H_(2)O_(2)production.Besides,the unique 3D nanostructure and surface hydrophobicity of IS/KCN facilitate the diffusion and transportation of O_(2)around the active centers,the energy barriers of O_(2)protonation and H_(2)O_(2)desorption steps are ef-fectively reduced over the composite.In addition,this system also exhibits excellent light harvesting ability and stability.This work provides a potential strategy to explore a sustainable H_(2)O_(2)photo-synthesis pathway through the design of heterojunctions with intimate interfaces and desired reac-tion thermodynamics and kinetics. 展开更多
关键词 Photocatalysis H_(2)O_(2)production K^(+)-doped g-C3N4 In2.77S4 S-scheme heterojunction
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Direct synthesis of nitrogen-doped mesoporous carbons for acetylene hydrochlorination 被引量:7
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作者 杨勇 蓝国钧 +1 位作者 王小龙 李瑛 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第8期1242-1248,共7页
Nitrogen‐doped ordered mesoporous carbon (N‐OMC) catalysts were directly synthesized using SBA‐15 as a hard template and sucrose as a carbon source. Urea, which was used as the nitrogen source, was carbonized wit... Nitrogen‐doped ordered mesoporous carbon (N‐OMC) catalysts were directly synthesized using SBA‐15 as a hard template and sucrose as a carbon source. Urea, which was used as the nitrogen source, was carbonized with sucrose. A 3.6 wt% nitrogen doping of the carbon framework was achieved, with more than 70%of the nitrogen incorporated as quaternary nitrogen species. Only 0.2 wt% nitrogen doping, with only 32.7% quaternary nitrogen incorporation was obtained in an N‐OMC catalyst (N‐OMC‐T) prepared using a two‐step post‐synthesis method. The acetylene hy‐drochlorination activities of N‐OMC catalysts prepared via the one‐step method were higher than that of the N‐OMC‐T catalyst because of the higher nitrogen loadings. 展开更多
关键词 ACETYLENE HYDROCHLORINATION Vinyl chloride MERCURY-FREE N-doped carbon
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Fabrication of porous g-C_3N_4 and supported porous g-C_3N_4 by a simple precursor pretreatment strategy and their efficient visible-light photocatalytic activity 被引量:6
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作者 曾振兴 李可心 +4 位作者 魏凯 戴玉华 颜流水 郭会琴 罗旭彪 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2017年第3期498-508,共11页
Porous g-C_3N_4 and supported porous g-C_3N_4 were fabricated for the first time by a simple strategy using pretreated melamine as a raw material and pretreated quartz rod as a substrate.The formation of a richly poro... Porous g-C_3N_4 and supported porous g-C_3N_4 were fabricated for the first time by a simple strategy using pretreated melamine as a raw material and pretreated quartz rod as a substrate.The formation of a richly porous microstructure can be attributed to the co-existence of different pore-fabricating units in the preparation system for porous g-C_3N_4.The richly porous microstructure endowed the as-prepared porous g-C_3N_4 with an excellent photocatalytic activity.The as-prepared supported porous g-C_3N_4 exhibited considerable stability because of the existence of chemical interaction between porous g-C_3N_4 and the quartz rod substrate.The photocatalytic activity of the supported porous g-C_3N_4 was competitive with that of porous g-C_3N_4 in powder form because neither the surface migration of photogenerated electrons nor the diffusion of the target organic pollutant were affected by the construction of the quartz rod reactor.The photocatalytic activity of the as-prepared porous g-C_3N_4 and supported porous g-C_3N_4 was preliminarily evaluated by the treatment of single-component organic wastewater under visible-light irradiation.Subsequently,the as-prepared porous g-C_3N_4 was further applied in conventional hydrogen evolution and a new system for simultaneous hydrogen evolution with organic-pollutant degradation.The hydrogen yield and degradation efficiency both increased with increasing photocatalytic activity of the as-prepared materials in the system for simultaneous hydrogen evolution with organic-pollutant degradation. 展开更多
关键词 Porous microstructure Graphitic carbon nitride SUBSTRATE Degradation Hydrogen evolution
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Structural and Optical Performance of GaN Thick Film Grown by HVPE
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作者 魏同波 马平 +5 位作者 段瑞飞 王军喜 李晋闽 刘喆 林郭强 曾一平 《Journal of Semiconductors》 EI CAS CSCD 北大核心 2007年第1期19-23,共5页
Thick GaN films were grown on GaN/sapphire template in a vertical HVPE reactor. Various material characterization techniques,including AFM, SEM, XRD, RBS/Channeling, CL, PL, and XPS, were used to characterize these Ga... Thick GaN films were grown on GaN/sapphire template in a vertical HVPE reactor. Various material characterization techniques,including AFM, SEM, XRD, RBS/Channeling, CL, PL, and XPS, were used to characterize these GaN epitaxial films. It was found that stepped/terraced structures appeared on the film surface,which were indicative of a nearly step-flow mode of growth for the HVPE GaN despite the high growth rate. A few hexagonal pits appeared on the surface, which have strong light emission. After being etched in molten KOH, the wavy steps disappeared and hexagonal pits with {1010} facets appeared on the surface. An EPD of only 8 ×10^6cm^-2 shows that the GaN film has few dislocations. Both XRD and RBS channeling indicate the high quality of the GaN thick films. Sharp band-edge emission with a full width at half maximum(FWHM)of 67meV was observed, while the yellow and infrared emissions were also found. These emissions are likely caused by native defects and C and O impurities. 展开更多
关键词 GAN HVPE CL RBS/channeling yellow emission infrared emission
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Enhanced photocatalytic H_2 production over dual-cocatalyst-modified g-C_3N_4 heterojunctions 被引量:8
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作者 Zong Li Yongning Ma +2 位作者 Xiaoyun Hu Enzhou Liu Jun Fan 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第3期434-445,共12页
Ag nanoparticles (NPs) were deposited on the surface of g-C3N4 (CN) by an in situ calcination method. NiS was successfully loaded onto the composites by a hydrothermal method. The results showed that the 10 wt%-NiS/1.... Ag nanoparticles (NPs) were deposited on the surface of g-C3N4 (CN) by an in situ calcination method. NiS was successfully loaded onto the composites by a hydrothermal method. The results showed that the 10 wt%-NiS/1.0 wt%-Ag/CN composite exhibits excellent photocatalytic H2 generation performance under solar-light irradiation. An H2 production rate of 9.728 mmol·g^-1·h^-1 was achieved, which is 10.82-, 3.45-, and 2.77-times higher than those of pure g-C3N4, 10 wt%-NiS/CN, and 1.0 wt%-Ag/CN composites, respectively. This enhanced photocatalytic H2 generation can be ascribed to the co-decoration of Ag and NiS on the surface of g-C3N4, which efficiently improves light harvesting capacity, photogenerated charge carrier separation, and photocatalytic H2 production kinetics. Thus, this study demonstrates an effective strategy for constructing excellent g-C3N4-related composite photocatalysts for H2 production by using different co-catalysts. 展开更多
关键词 PHOTOCATALYSIS Photocatalytic H2 generation g-C3N4 Ag NIS
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Preparation of N‐vacancy‐doped g‐C_3N_4 with outstanding photocatalytic H_2O_2 production ability by dielectric barrier discharge plasma treatment 被引量:11
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作者 Xuhe Li Jian Zhang +4 位作者 Feng Zhou Hongliang Zhang Jin Bai Yanjuan Wang Haiyan Wang 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第6期1090-1098,共9页
Dielectric barrier discharge(DBD) plasma is considered to be a promising method to synthesize solid catalysts. In this work, DBD plasma was used to synthesize a nitrogen‐vacancy‐doped g‐C3N4 catalyst in situ for ... Dielectric barrier discharge(DBD) plasma is considered to be a promising method to synthesize solid catalysts. In this work, DBD plasma was used to synthesize a nitrogen‐vacancy‐doped g‐C3N4 catalyst in situ for the first time. X‐ray diffraction, N2 adsorption, ultraviolet–visible spectroscopy, scanning electron microscopy, transmission electron microscopy, X‐ray photoelectron spectrosco‐py, electrochemical impedance spectroscopy, electron paramagnetic resonance, O2 tempera‐ture‐programmed desorption, and photoluminescence were used to characterize the obtained cat‐alysts. The photocatalytic H2O2 production ability of the as‐prepared catalyst was investigated. The results show that plasma treatment influences the morphology, structure, and optical properties of the as‐prepared catalyst. Nitrogen vacancies are active centers, which can adsorb reactant oxygen molecules, trap photoelectrons, and promote the transfer of photoelectrons from the catalyst to the adsorbed oxygen molecules for the subsequent reduction reaction. This work provides a new strat‐egy for synthesizing g‐C3N4‐based catalysts. 展开更多
关键词 Dielectric BARRIER discharge plasma Graphitic carbonnitride H2O2 productionNitrogen VACANCIES PHOTOCATALYSIS
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Wheat flour-derived N-doped mesoporous carbon extrudes as an efficient support for Au catalyst in acetylene hydrochlorination 被引量:4
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作者 Jie Liu Guojun Lan +2 位作者 Yiyang Qiu Xiaolong Wang Ying Li 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第10期1664-1671,共8页
We recently reported an N‐doped mesoporous carbon(N‐MC)extrudate,with major quaternary N species,prepared by a cheap and convenient method through direct carbonization of wheat flour with silica,which has excellent ... We recently reported an N‐doped mesoporous carbon(N‐MC)extrudate,with major quaternary N species,prepared by a cheap and convenient method through direct carbonization of wheat flour with silica,which has excellent catalytic performance in acetylene hydrochlorination.Herein,we examined the activity of Au supported on N‐MC(Au/N‐MC)and compared it with that of Au supported on nitrogen‐free mesoporous carbon(Au/MC).The acetylene conversion of Au/N‐MC was 50%at 180°C with an acetylene space velocity of 600 h–1 and VHCl/VC2H2 of 1.1,which was double the activity of Au/MC(25%).The introduced nitrogen atoms acted as anchor sites that stabilized the Au3+species and inhibited the reduction of Au3+to Au0 during the preparation of Au/N‐MC catalysts. 展开更多
关键词 Au catalyst Mercury free catalyst Acetylene hydrochlorination N doped mesoporous carbon
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High selectivity to p-chloroaniline in the hydrogenation of p-chloronitrobenzene on Ni modified carbon nitride catalyst 被引量:2
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作者 符滕 胡佩 +5 位作者 王涛 董珍 薛念华 彭路明 郭学峰 丁维平 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2015年第11期2030-2035,共6页
A nanocomposite composed of Ni modified carbon nitride was synthesized and used in the hydro- genation of p-chloronitrobenzene. H/D exchange demonstrated that the hydrogen chemisorbed on the surface of this nanocompos... A nanocomposite composed of Ni modified carbon nitride was synthesized and used in the hydro- genation of p-chloronitrobenzene. H/D exchange demonstrated that the hydrogen chemisorbed on the surface of this nanocomposite catalyst had a hydrogen atom density of 0.65/nm2. It was active for hydrogenation but its activity was inferior to the hydrogen adsorbed on a Ni/Al2O3 catalyst. Catalytic tests showed that this catalyst possessed a lower activity than Ni/AhO3 but the selectivity towards p-chloroaniline was above 99.9%. Even at high conversion, the catalyst maintained high selectivity, which was attributed to the unique surface property of the catalyst and the absence of a site for the adsorption ofp-chloronitrobenzene, which prevents the C-Cl bond from breaking. 展开更多
关键词 Hydrogenationp-Chloronitrobenzene Carbon nitride NickelSelectivity
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Study on Chemisorption and Desorption of Hydrogen and Nitrogen on Ru-based Ammonia Synthesis Catalyst 被引量:4
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作者 祝一锋 李小年 +2 位作者 周春晖 高冬梅 刘化章 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2003年第1期15-18,共4页
The effects of promoters K, Ba, Sm on the chemisorption and desorption of hydrogen and nitrogen, dispersion of metallic Ru. and catalytic activity of active carbon (AC) supported ruthenium catalyst for ammonia synthes... The effects of promoters K, Ba, Sm on the chemisorption and desorption of hydrogen and nitrogen, dispersion of metallic Ru. and catalytic activity of active carbon (AC) supported ruthenium catalyst for ammonia synthesis have been studied by means of pulse chromatography, temperature-programmed desorption, and activity test. Promoters K, Ba and Sm increased the activity of Ru/AC catalysts for ammonia synthesis significantly, and particularly, potassium exhibited the best promotion on the activity because of the strong electronic donation to metallic Ru. Much higher activity can be obtained for Ru/AC catalyst with binary or triple promoters. The activity of Ru/AC catalyst is dependent on the adsorption of hydrogen and nitrogen. The high activity of catalyst could be ascribed to strong dissociation of nitrogen on the catalyst surface. Strong adsorption of hydrogen would inhibit the adsorption of nitrogen, resulted in decrease of the catalytic activity. Ru/AC catalyst promoted by Sm2O3 shows the best dispersion of metallic Ru, since the partly reduced SmOx on the surface modifies the morphology of active sites and favors the dispersion of metallic Ru. The activity of Ru/AC catalysts is in accordance to the corresponding amount of nitrogen chemisorption and the desorption activation energy of nitrogen. The desorption activation energy for nitrogen decreases in the order of Ru>Ru-Ba>Ru-Sm>Ru-Ba-Sm>Ru-K>Ru-K-Sm>Ru-K-Ba>Ru-K-Ba-Sm, just opposite to the order of catalytic activity, suggesting that the ammonia synthesis over Ru-based catalyst is controlled by the step of dissociation of nitrogen. 展开更多
关键词 RUTHENIUM CATALYST ammonia synthesis CHEMISORPTION DESORPTION
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Electronic interaction between single Pt atom and vacancies on boron nitride nanosheets and its influence on the catalytic performance in the direct dehydrogenation of propane 被引量:7
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作者 Xiaoying Sun Meijun Liu +2 位作者 Yaoyao Huang Bo Li Zhen Zhao 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第6期819-825,共7页
The electronic metal-support interaction(EMSI)is one of most intriguing phenomena in heterogeneous catalysis.In this work,this subtle effect is clearly demonstrated by density functional theory(DFT)calculations of sin... The electronic metal-support interaction(EMSI)is one of most intriguing phenomena in heterogeneous catalysis.In this work,this subtle effect is clearly demonstrated by density functional theory(DFT)calculations of single Pt atom supported on vacancies in a boron nitride nanosheet.Moreover,the relation between the EMSI and the performance of Pt in propane direct dehydrogenation(PDH)is investigated in detail.The charge state and partial density of states of single Pt atom show distinct features at different anchoring positions,such as boron and nitrogen vacancies(Bvac and Nvac,respectively).Single Pt atom become positively and negatively charged on Bvac and Nvac,respectively.Therefore,the electronic structure of Pt can be adjusted by rational deposition on the support.Moreover,Pt atoms in different charge states have been shown to have different catalytic abilities in PDH.The DFT calculations reveal that Pt atoms on Bvac(Pt-Bvac)have much higher reactivity towards reactant/product adsorption and C–H bond activation than Pt supported on Nvac(Pt-Nvac),with larger adsorption energy and lower barrier along the reaction pathway.However,the high reactivity of Pt-Bvac also hinders propene desorption,which could lead to unwanted deep dehydrogenation.Therefore,the results obtained herein suggest that a balanced reactivity for C–H activation in propane and propene desorption is required to achieve optimum yields.Based on this descriptor,a single Pt atom on a nitrogen vacancy is considered an effective catalyst for PDH.Furthermore,the deep dehydrogenation of the formed propene is significantly suppressed,owing to the large barrier on Pt-Nvac.The current work demonstrates that the catalytic properties of supported single Pt atoms can be tuned by rationally depositing them on a boron nitride nanosheet and highlights the great potential of single-atom catalysis in the PDH reaction. 展开更多
关键词 PROPANE Direct dehydrogenation Platinum Boron nitride Single atom catalysis Density functional theory Electronic metel-support interaction
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Defect‐rich BN‐supported Cu with superior dispersion for ethanol conversion to aldehyde and hydrogen 被引量:2
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作者 Shi‐Qun Cheng Xue‐Fei Weng +6 位作者 Qing‐Nan Wang Bai‐Chuan Zhou Wen‐Cui Li Ming‐Run Li Lei He Dong‐Qi Wang An‐Hui Lu 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第4期1092-1100,共9页
Copper‐based heterogeneous catalysts commonly exhibit uncontrolled growth of copper species under reaction conditions because of the low Hüttig temperature(surface mobility of atoms)and Tamman temperature(bulk m... Copper‐based heterogeneous catalysts commonly exhibit uncontrolled growth of copper species under reaction conditions because of the low Hüttig temperature(surface mobility of atoms)and Tamman temperature(bulk mobility)for copper at just 134 and 405°C,respectively.Herein,we report the use of defect‐enriched hexagonal boron nitride nanosheets(BNSs)as a support to anchor the Cu species,which resulted in superior dispersion of the Cu species.The obtained Cu/BNS catalyst was highly stable for ethanol dehydrogenation,with a high selectivity of 98%for producing acetaldehyde and an exceptionally high acetaldehyde productivity of 7.33 g_(AcH) g_(cat)^(‒1) h^(‒1) under a weight hourly space velocity of 9.6 g_(EtOH) g_(cat)^(‒1) h^(‒1).The overall performance of our designed catalyst far exceeded that of most reported heterogeneous catalysts in terms of the stability of the Cu species and the yield of acetaldehyde in this reaction.The hydroxyl groups at the defect edges of BNS were responsible for the stabilization of the copper species,and the metal‐support interaction was reinforced through charge transfer,as evidenced by coupling atomic resolution images with probe molecule infrared spectroscopy and X‐ray photoelectron spectroscopy.A designed in situ diffuse reflectance infrared Fourier transform spectroscopy study of ethanol/acetaldehyde adsorption further revealed that Cu/BNS favored ethanol adsorption while suppressing acetaldehyde adsorption and further side reactions.This study demonstrates a new method for designing highly dispersed Cu‐based catalysts with high durability. 展开更多
关键词 Ethanol dehydrogenation Copper Boron nitride nanosheet Superior dispersion In situ DRIFT
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Palladium nanoparticles assembled on titanium nitride for enhanced electrochemical hydrodechlorination of 2,4-dichlorophenol in water 被引量:6
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作者 Wenyang Fu Kaifeng Wang +5 位作者 Xiaoshu Lv Hailu Fu Xingan Dong Ling Chen Xianming Zhang Guangming Jiang 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第4期693-700,共8页
We report a one‐pot surfactant‐free wet‐chemical reduction approach to the synthesis of palladium/titanium nitride(Pd/TiN)and Pd/carbon(Pd/C)composites,in which^5 nm Pd NPs were uniformly dispersed on TiN or C.In t... We report a one‐pot surfactant‐free wet‐chemical reduction approach to the synthesis of palladium/titanium nitride(Pd/TiN)and Pd/carbon(Pd/C)composites,in which^5 nm Pd NPs were uniformly dispersed on TiN or C.In terms of catalytic performance,Pd/TiN showed enhanced efficiency and stability compared with those of Pd/C and bare TiN in the electrocatalytic hydrodechlorination(EHDC)reaction of 2,4‐dichlorophenol(2,4‐DCP)in aqueous solution.The superior performance of Pd/TiN arises from the promotion effect of TiN.Strong metal‐support interactions modified the electronic structure of Pd,which optimized generation of H*ads and 2,4‐DCP adsorption/activation.The cathode potential plays a vital role in controlling the EHDC efficiency and the product distribution.A working potential of?0.80 V was shown to be optimal for achieving the highest EHDC efficiency and maximizing conversion of 2,4‐DCP to phenol(P).Our studies of the reaction pathway show that EHDC of 2,4‐DCP on Pd/TiN proceeded by 2,4‐DCP→p‐chlorophenol(p‐CP),o‐chlorophenol(o‐CP)→P;however,Pd/TiN presented little selectivity for cleavage of p‐C‐Cl vs o‐C‐Cl.This work presents a new approach to enhancing Pd performance towards EHDC through the effects of a support.The strategy demonstrated here could also be extended to design highly efficient catalysts for other hydrogenation reactions. 展开更多
关键词 HYDRODECHLORINATION ELECTROLYSIS PALLADIUM Titanium nitride Environmental remediation
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Highly crystalline carbon nitride hollow spheres with enhanced photocatalytic performance 被引量:15
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作者 Yang Li Dainan Zhang +1 位作者 Jiajie Fan Quanjun Xiang 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第4期627-636,共10页
Graphitic carbon nitride(g-C_(3)N_(4))has emerged as a remarkably promising photocatalyst for addressing environmental and energy issues;however,it exhibits only moderate photocatalytic activity because of its low spe... Graphitic carbon nitride(g-C_(3)N_(4))has emerged as a remarkably promising photocatalyst for addressing environmental and energy issues;however,it exhibits only moderate photocatalytic activity because of its low specific surface area and high recombination of carriers.Preparation of crystalline g-C_(3)N_(4) by the molten salt method has proven to be an effective method to improve the photocatalytic activity.However,crystalline g-C_(3)N_(4) prepared by the conventional molten salt method exhibits a less regular morphology.Herein,highly crystalline g-C_(3)N_(4) hollow spheres(CCNHS)were successfully prepared by the molten salt method using cyanuric acid-melamine as a precursor.The higher crystallization of the CCNHS samples not only repaired the structural defects at the surface of the CCNHS samples but also established a built-in electric field between heptazine-based g-C_(3)N_(4) and triazine-based g-C_(3)N_(4).The hollow structure improved the level of light energy utilization and increased the number of active sites for photocatalytic reactions.Because of the above characteristics,the as-prepared CCNHS samples simultaneously realized photocatalytic hydrogen evolution with the degradation of the plasticizer bisphenol A.This research offers a new perspective on the structural optimization of supramolecular self-assembly. 展开更多
关键词 CRYSTALLINE Hollow spheres Graphitic carbon nitride Photocatalytic hydrogen evolution Photocatalytic degradation PLASTICIZER
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An efficient strategy for photocatalytic hydrogen peroxide production over oxygen-enriched graphitic carbon nitride with sodium phosphate 被引量:2
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作者 Yu Zhang Ling Zhang +4 位作者 Di Zeng Wenjing Wang Juxue Wang Weimin Wang Wenzhong Wang 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第10期2690-2698,共9页
Photocatalytic hydrogen peroxide(H_(2)O_(2))production is a promising strategy to replace the traditional production processes;however,the inefficient H_(2)O_(2) productivity limits its application.In this study,oxyge... Photocatalytic hydrogen peroxide(H_(2)O_(2))production is a promising strategy to replace the traditional production processes;however,the inefficient H_(2)O_(2) productivity limits its application.In this study,oxygen-rich g-C_(3)N_(4) with abundant nitrogen vacancies(OCN)was synthesized for photocatalytic H_(2)O_(2) production.X-ray photoelectron spectroscopy and Fourier-transform infrared spectroscopy indicated that oxygen-containing functional groups(–COOH and C–O–C)were obtained.Electron paramagnetic resonance confirmed the successful introduction of nitrogen vacancies.OCN exhibited efficient photocatalytic H_(2)O_(2) production performance of 1965μmol L^(−1) h^(−1) in air under visible-light irradiation.The high H_(2)O_(2) production was attributed to the enhanced adsorption of oxygen,enlarged specific surface area,and promoted carrier separation.An increased H_(2)O_(2) production rate(5781μmol L^(−1) h^(−1))was achieved in a Na_(3)PO_(4) solution.The improved performance was attributed to the changed reactive oxygen species.Specifically,the adsorbed PO_(4)^(3−) on the surface of the OCN promoted the transfer of holes to the catalyst surface.•O_(2)−obtained by O_(2) reduction reacted with adjacent holes to generate 1O_(2),which could efficiently generate H_(2)O_(2) with isopropanol.Additionally,PO_(4)^(3−),as a stabilizer,inhibited the decomposition of H_(2)O_(2). 展开更多
关键词 PHOTOCATALYSIS Hydrogen peroxide production Graphitic carbon nitride Singlet oxygen Sodium phosphate
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Oxygen and nitrogen-doped metal-free carbon catalysts for hydrochlorination of acetylene 被引量:6
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作者 Tongtong Zhang Jia Zhao +3 位作者 Jiangtao Xu Jinhui Xu Xiaoxia Di Xiaonian Li 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2016年第4期484-490,共7页
Activated carbon was tested as metal-free catalyst for hydrochlorination of acetylene in order to circumvent the problem of environment pollution caused by mercury and high cost by noble metals. Oxygen-doped and nitro... Activated carbon was tested as metal-free catalyst for hydrochlorination of acetylene in order to circumvent the problem of environment pollution caused by mercury and high cost by noble metals. Oxygen-doped and nitrogen-doped activated carbons were prepared and characterized by XPS, TPD and N2 physisorption methods. The influences of the surface functional groups on the catalytic performance were discussed base on these results. Among all the samples tested, a nitrogen-doped sample, AC-n-US00, exhibited the best performance, the acety- lene conversion being 92% and vinyl chloride selectivity above 99% at 240 ~C and C2H2 hourly space velocity 30 h- 1. Moreover, the AC-n-US00 catalyst exhibited a stable performance during a 200 h test with a conversion of acetylene higher than 76% at 210 ~C at a C2H2 hourly space velocity 50 h 1. In contrary, oxygen-doped catalyst had lower catalytic activities. A linear relationship between the amount of pyrrolic-N and quaternary-N species and the catalytic activity was observed, indicating that these nitrogen-doped species might be the active sites and the key in tuning the catalytic performance. It is also found that the introduction of nitrogen species into the sample could significantly increase the adsorption amount of acetylene. The deactivation of nitrogen- doped activated carbon might be caused by the decrease of the accessibility to or the total amount of active sites. 展开更多
关键词 Acetylene hydrochlorinationActivated carbonSurface chemistryOxygenated groupNitrogen-doped
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Gold/monolayer graphitic carbon nitride plasmonic photocatalyst for ultrafast electron transfer in solar-to-hydrogen energy conversion 被引量:3
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作者 Zhao Mo Hui Xu +7 位作者 Zhigang Chen Xiaojie She Yanhua Song Pengcheng Yan Yuanguo Xu Yucheng Lei Shouqi Yuan Huaming Li 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第4期760-770,共11页
Gold(Au)plasmonic nanoparticles were grown evenly on monolayer graphitic carbon nitride(g‐C3N4)nanosheets via a facile oil‐bath method.The photocatalytic activity of the Au/monolayer g‐C3N4 composites under visible... Gold(Au)plasmonic nanoparticles were grown evenly on monolayer graphitic carbon nitride(g‐C3N4)nanosheets via a facile oil‐bath method.The photocatalytic activity of the Au/monolayer g‐C3N4 composites under visible light was evaluated by photocatalytic hydrogen evolution and environmental treatment.All of the Au/monolayer g‐C3N4 composites showed better photocatalytic performance than that of monolayer g‐C3N4 and the 1%Au/monolayer g‐C3N4 composite displayed the highest photocatalytic hydrogen evolution rate of the samples.The remarkable photocatalytic activity was attributed largely to the successful introduction of Au plasmonic nanoparticles,which led to the surface plasmon resonance(SPR)effect.The SPR effect enhanced the efficiency of light harvesting and induced an efficient hot electron transfer process.The hot electrons were injected from the Au plasmonic nanoparticles into the conduction band of monolayer g‐C3N4.Thus,the Au/monolayer g‐C3N4 composites possessed higher migration and separation efficiencies and lower recombination probability of photogenerated electron‐hole pairs than those of monolayer g‐C3N4.A photocatalytic mechanism for the composites was also proposed. 展开更多
关键词 Monolayer g‐C3N4 Au plasmonic nanoparticle Photocatalytic hydrogen evolution Hot electron Au/monolayer g‐C3N4
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In situ synthesis of Fe-N-C catalysts from cellulose for hydrogenation of nitrobenzene to aniline 被引量:4
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作者 Hao Wang Xiaohao Liu +2 位作者 Guangyue Xu Ziwei Guo Ying Zhang 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第10期1557-1565,共9页
Owing to Fe being the most abundant and least expensive transition metal on the earth,the utilization of Fe-based catalysts for catalytic hydrogenation has attracted worldwide attention.In this work,a series of N-dope... Owing to Fe being the most abundant and least expensive transition metal on the earth,the utilization of Fe-based catalysts for catalytic hydrogenation has attracted worldwide attention.In this work,a series of N-doped C supported Fe catalysts(Fe-N-C)were prepared by co-pyrolysis of cellulose and ferric chloride under ammonia atmosphere.Characterization methods such as elemental analysis,atomic absorption spectroscopy,nitrogen adsorption-desorption isotherms,transmission electron microscopy,high-resolution transmission electron microscopy,X-ray diffraction,and X-ray photoelectron spectroscopy were carried out to explore the physicochemical properties of the catalysts.Using hydrogenation of nitrobenzene as a model reaction,the catalysts prepared at different pyrolysis temperatures displayed different activities.Fe-N-C-700 exhibited the best activity among these catalysts,with the yield of aniline being up to 98.0%under 5 MPa H2 at 120℃ after 12 h.Combined with the results of catalyst characterization and comparative tests,the transformation of Fe species and the generation of N-doped C,especially graphitized N-doped C,in the catalyst may be the main factors affecting the activity.A kinetic study was carried out and the apparent activation energy was obtained as 31.53 kJ/mol.The stability of the catalyst was also tested and no significant decrease in the activity was observed after 5 runs. 展开更多
关键词 CO-PYROLYSIS Iron NITROGEN-DOPED Carbon HYDROGENATION
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The embedded CuInS2 into hollow-concave carbon nitride for photocatalytic H2O splitting into H2 with S-scheme principle 被引量:15
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作者 Jinhua Luo Zhexing Lin +2 位作者 Yan Zhao Shujuan Jiang Shaoqing Song 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2020年第1期122-130,共9页
It is still a great challenge to effectively optimize the electronic structure of photocatalysts for the sustainable and efficient conversion of solar energy to H2 energy.To resolve this issue,we report on the optimiz... It is still a great challenge to effectively optimize the electronic structure of photocatalysts for the sustainable and efficient conversion of solar energy to H2 energy.To resolve this issue,we report on the optimization of the electronic structure of hollow-concave carbon nitride(C3N4)by deviating the sp2-hybridized structure of its tri-s-triazine component from the two-dimensional plane.The embedded CuInS2 into C3N4(CuInS2@C3N4)demonstrates an increased light-capturing capability and the promoted directional transfer of the charge carrier.Research results reveal that the hollow structure with an apparent potential difference between the concave and convex C3N4 drives the directional transfer of the photoinduced electrons from the Cu 2p orbital of CuInS2 to the N 1s orbital of C3N4 with the S-scheme principle.The H2 evolution efficiency over CuInS2@C3N4 is up to 373μmol?h^-1 g^-1 under visible irradiation,which is 1.57 and 1.35 times higher than those over the bulk g-C3N4 with 1 wt%Pt(238μmol?h^-1 g^-1)and g-C3N4 with 3 wt%Pd(276μmol?h^-1 g^-1),respectively.This suggests that the apparent potential difference of the hollow C3N4 results in an efficient reaction between the photogenerated electrons and H2O.This work supplies a new strategy for enhancing the sustainable solar conversion performance of carbon nitride,which can also be suitable for other semiconductors. 展开更多
关键词 Hollow carbon nitride Hydrogen evolution Solar light absorption Directional charge transfer Apparent potential difference
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MXenes as noble-metal-alternative co-catalysts in photocatalysis 被引量:7
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作者 Kaining Li Sushu Zhang +2 位作者 Yuhan Li Jiajie Fan Kangle Lv 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第1期3-14,共12页
Photocatalysis has become a focal point in research as a clean and sustainable technology with the potential to solve environmental problems and energy crises.The loading of noble-metal co-catalysts can substantially ... Photocatalysis has become a focal point in research as a clean and sustainable technology with the potential to solve environmental problems and energy crises.The loading of noble-metal co-catalysts can substantially improve the photocatalytic efficiency of semiconductors.Because the high cost and scarcity of noble metals markedly limit their large-scale applications,finding a noble-metal-alternative co-catalyst is crucial.MXene,a novel 2D transition metal material,has attracted considerable attention as a promising substitute for noble metal co-catalysts owing to its cost-efficiency,unique 2D layered structure,and excellent electrical,optical,and thermodynamic properties.This review focuses on the latest advancements in research on MXenes as co-catalysts in relatively popular photocatalytic applications(hydrogen production,CO2 reduction,nitrogen fixation,and organic pollutant oxidation).The synthesis methods and photocatalytic mechanisms of MXenes as co-catalysts are also summarized according to the type of MXene-based material.Finally,the crucial opportunities and challenges in the prospective development of MXene-based photocatalysts are outlined.We emphasize that modern techniques should be used to demonstrate the effects of MXenes on photocatalysis and that the photocatalytic activity of MXene-based photocatalysts can be further improved using defective engineering and recent phenomena such as the localized surface plasmon resonance effect and single-atom catalysis. 展开更多
关键词 MXenes Photocatalytic degradation Hydrogen production CO2 reduction Nitrogen fixation
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Pyrrolidine dithiocarbamate reduces ischemia-reperfusion injury of the small intestine 被引量:8
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作者 Ismail H Mallick Wen-Xuan Yang +1 位作者 Marc C Winslet Alexander M Seifalian 《World Journal of Gastroenterology》 SCIE CAS CSCD 2005年第46期7308-7313,共6页
AIM: To evaluate whether pyrrolidine dithiocarbamate (PDTC), an enhancer of HO production, attenuates intestinal IR injury. METHODS: Eighteen male rats were randomly allocated into three groups: (a) sham; (b)... AIM: To evaluate whether pyrrolidine dithiocarbamate (PDTC), an enhancer of HO production, attenuates intestinal IR injury. METHODS: Eighteen male rats were randomly allocated into three groups: (a) sham; (b) IR, consisting of 30 min of intestinal ischemia, followed by 2-h period of reperfusion; and (c) PDTC treatment before IR. Intestinal microvascular perfusion (IMP) was monitored continuously by laser Doppler flowmetry. At the end of the reperfusion, serum samples for lactate dehydrogenase (LDH) levels and biopsies of ileum were obtained. HO activity in the ileum was assessed at the end of the reperfusion period. RESULTS: At the end of the reperfusion in the IR group, IMP recovered partially to 42.5% of baseline (P〈0.05 vs sham), whereas PDTC improved IMP to 67.3% of baseline (P〈0.01 vs IR). There was a twofold increase in HO activity in PDTC group (2 062.66±106.11) as compared to IR (842.3±85.12) (P〈0.001). LDH was significantly reduced (P〈0.001) in PDTC group (585.6±102.4) as compared to IR group (1 973.8±306.5). Histological examination showed that the ileal mucosa was significantly less injured in PDTC group as compared with IR group. CONCLUSION: Our study demonstrates that PDTC improves the IMP and attenuates IR injury of the intestine possibly via HO production. Additional studies are warranted to evaluate the clinical efficacy of PDTC in the prevention of IR injury of the small intestine. 展开更多
关键词 INTESTINE Ischemia-reperfusion injury Heme oxygenase PYRROLIDINE
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