The development of anode materials with high rate capability and long charge-discharge plateau is the key to improve per-formance of lithium-ion capacitors(LICs).Herein,the porous graphitic carbon(PGC-1300)derived fro...The development of anode materials with high rate capability and long charge-discharge plateau is the key to improve per-formance of lithium-ion capacitors(LICs).Herein,the porous graphitic carbon(PGC-1300)derived from a new triply interpenetrated co-balt metal-organic framework(Co-MOF)was prepared through the facile and robust carbonization at 1300°C and washing by HCl solu-tion.The as-prepared PGC-1300 featured an optimized graphitization degree and porous framework,which not only contributes to high plateau capacity(105.0 mAh·g^(−1)below 0.2 V at 0.05 A·g^(−1)),but also supplies more convenient pathways for ions and increases the rate capability(128.5 mAh·g^(−1)at 3.2 A·g^(−1)).According to the kinetics analyses,it can be found that diffusion regulated surface induced capa-citive process and Li-ions intercalation process are coexisted for lithium-ion storage.Additionally,LIC PGC-1300//AC constructed with pre-lithiated PGC-1300 anode and activated carbon(AC)cathode exhibited an increased energy density of 102.8 Wh·kg^(−1),a power dens-ity of 6017.1 W·kg^(−1),together with the excellent cyclic stability(91.6%retention after 10000 cycles at 1.0 A·g^(−1)).展开更多
Common strategies for catalytic graphitization of biochar into graphitic porous carbon(GPC)still face great challenges,such as the realization of simple procedures,energy conservation,and green processes.Controlling o...Common strategies for catalytic graphitization of biochar into graphitic porous carbon(GPC)still face great challenges,such as the realization of simple procedures,energy conservation,and green processes.Controlling over the graphitization degree and pore structure of biochar is the key to its structural diversification.Herein,a clean and energy-efficient method is developed to synthesize adjustable graphitic degree and structure porosity GPC from rice husk-based carbon(RHC)at a relatively low temperature of 800–1000°C with environment-benign organometallic catalyst ethylenediaminetetraacetic acid ferric sodium salt(EDTA-iron)and the recovery ratio of catalyst is as high as 97%.The formed by the organic ligands of EDTA-iron facilitates the etching of RHC surface and pore by iron,resulting in highly graphitized and developed porous GPCs.The pore structure and graphitization degree of GPCs can be adjusted by altering the catalyst loading,temperature,and holding time.The catalyst EDTA-iron with a lower concentration mainly plays the role of etching,which promotes the formation of porous carbon with larger surface area(SBET=1187.2 m^(2)·g^(-1)).The catalyst with higher concentration mainly plays the role of catalyzing graphitization and promotes the obtaining of graphitic carbon with high graphitization degree(ID/IG=0.19).The mechanism of EDTA-iron catalyzed graphitization of RHC is explored by the comprehensive analysis of BET,XRD,Raman,TEM and TGA.This research not only provides an efficient method for the preparation of high-quality biomass-based graphite carbon,but also provides a feasible method for the preparation of biomass-based porous carbon.展开更多
Lithium-ion hybrid supercapacitors(Li-HSCs) and dual-ion batteries(DIBs) are two types of energy storage devices that have attracted extensive research interest in recent years. Li-HSCs and DIBs have similarities in d...Lithium-ion hybrid supercapacitors(Li-HSCs) and dual-ion batteries(DIBs) are two types of energy storage devices that have attracted extensive research interest in recent years. Li-HSCs and DIBs have similarities in device structure, tendency for ion migration, and energy storage mechanisms at the negative electrode. However, these devices have differences in energy storage mechanisms and working potentials at the positive electrode. Here, we first realize the integration of a Li-HSC and a DIB to form a dual-ion hybrid supercapacitor(DIHSC), by employing mesocarbon microbead(MCMB)-based porous graphitic carbon(PGC) with a partially graphitized structure and porous structure as a positive electrode material. The MCMB-PGC-based DIHSC exhibits a novel dual-ion battery-capacitor hybrid mechanism: it exhibits excellent electronic double-layer capacitor(EDLC) behavior like a Li-HSC in the low-middle wide potential range and anion intercalation/de-intercalation behavior like a DIB in the high-potential range. Two types of mechanisms are observed in the electrochemical characterization process, and the energy density of the new DIHSC is significantly increased.展开更多
A hierarchical micro-nano porous carbon material (MNC) was prepared using expanded graphite (EG), sucrose, and phosphoric acid as raw materials, followed by sucrose-phosphoric acid solution impregnation, solidificatio...A hierarchical micro-nano porous carbon material (MNC) was prepared using expanded graphite (EG), sucrose, and phosphoric acid as raw materials, followed by sucrose-phosphoric acid solution impregnation, solidification, carbonization and activation. Nitrogen adsorption and mercury porosimetry show that mixed nanopores and micropores coexist in MNC with a high specific surface area of 1978 m2·g-1 and a total pore volume of 0.99 cm3·g-1. In addition, the MNC is found to consist of EG and activated carbon with the latter deposited on the interior and the exterior surfaces of the EG pores. The thickness of the activated carbon layer is calculated to be about one hundred nanometers and is further confirmed by scanning electron microscope (SEM) and transmission election microscope (TEM). A maximum static phenol adsorption of 241.2 mg·g-1 was obtained by using MNC, slightly higher than that of 220.4 mg·g-1 by using commercial activated carbon (CAC). The phenol adsorption kinetics were investigated and the data fitted well to a pseudo-second-order model. Also, an intra-particle diffusion mechanism was proposed. Furthermore, it is found that the dynamic adsorption capacity of MNC is nearly three times that of CAC. The results suggest that the MNC is a more efficient adsorbent than CAC for the removal of phenol from aqueous solution.展开更多
The active site amount of photocatalysts,being the key factors in photocatalytic reactions,directly affects the photocatalytic performance of the photocatalyst.Pristine graphitic carbon nitride(g‐C_(3)N_(4))exhibits ...The active site amount of photocatalysts,being the key factors in photocatalytic reactions,directly affects the photocatalytic performance of the photocatalyst.Pristine graphitic carbon nitride(g‐C_(3)N_(4))exhibits moderate photocatalytic activity due to insufficient active sites.In this study,cyano‐modified porous g‐C_(3)N_(4)nanosheets(MCN‐0.5)were synthesized through molecular self‐assembly and alkali‐assisted strategies.The cyano group acted as the active site of the photocatalytic reaction,because the good electron‐withdrawing property of the cyano group promoted carrier separation.Benefiting from the effect of the active sites,MCN‐0.5 exhibited significantly enhanced photocatalytic activity for CO2 reduction under visible light irradiation.Notably,the photocatalytic activity of MCN‐0.5 was significantly reduced when the cyano groups were removed by hydrochloric acid(HCl)treatment,further verifying the role of cyano groups as active sites.The photoreduction of Pt nanoparticles provided an intuitive indication that the introduction of cyano groups provided more active sites for the photocatalytic reaction.Furthermore,the controlled experiments showed that g‐C_(3)N_(4)grafted with cyano groups using melamine as the precursor exhibited enhanced photocatalytic activity,which proved the versatility of the strategy for enhancing the activity of g‐C_(3)N_(4)via cyano group modification.In situ diffuse reflectance infrared Fourier transform spectroscopy and theoretical calculations were used to investigate the mechanism of enhanced photocatalytic activity for CO2 reduction by cyano‐modified g‐C_(3)N_(4).This work provides a promising route for promoting efficient solar energy conversion by designing active sites in photocatalysts.展开更多
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
A series of highly dispersed platinum‐deposited porous g‐C3N4 (Pt/pg‐C3N4) were successfully fabricated by a simple in situ photoreduction strategy using chloroplatinic acid and porous g‐C3N4 as precursors. Porou...A series of highly dispersed platinum‐deposited porous g‐C3N4 (Pt/pg‐C3N4) were successfully fabricated by a simple in situ photoreduction strategy using chloroplatinic acid and porous g‐C3N4 as precursors. Porous g‐C3N4 was fabricated by a pretreatment strategy using melamine as a raw material.The morphology, porosity, phase, chemical structure, and optical and electronic properties ofas‐prepared Pt/pg‐C3N4 were characterized. The photocatalytic activity of as‐prepared Pt/pg‐C3N4was preliminarily evaluated by the degradation of aqueous azo dyes methyl orange under visible light irradiation. The as‐prepared Pt/pg‐C3N4 were further applied to the degradation and mineralization of aqueous 4‐fluorophenol. The recyclability of Pt/pg‐C3N4 was evaluated under four consecutive photocatalytic runs.展开更多
Graphitic carbons with reasonable pore volume and appropriate graphitization degree can provide efficient Li+/electrolyte-transfer channels and ameliorate the sluggish dynamic behavior of battery-type carbon negative ...Graphitic carbons with reasonable pore volume and appropriate graphitization degree can provide efficient Li+/electrolyte-transfer channels and ameliorate the sluggish dynamic behavior of battery-type carbon negative electrode in lithium-ion capacitors(LICs).In this work,onion-like graphitic carbon materials are obtained by using carbon quantum dots as precursors after sintering,and the effects of alkali metal salts on the structure,morphology and performance of the samples are focused.The results show that alkali metal salts as activator can etch graphitic carbons,and the specific surface area and pore size distribution are intimately related to the description of the alkali metal salt.Moreover,it also affects the graphitization degree of the materials.The porous graphitic carbons(SGCs)obtained by NaCl activation exhibit high specific surface area(77.14 m^(2)·g^(-1))and appropriate graphitization degree.It is expectable that the electrochemical performance for lithium-ions storage can be largely promoted by the smart combination of catalytic graphitization and pores-creating strategy.High-performance LICs(S-GCs//AC LICs)are achieved with high energy density of 92 Wh·kg^(-1)and superior rate capability(66.3 Wh·kg^(-1)at10 A·g^(-1))together with the power density as high as10020.2 W·kg^(-1).展开更多
Aberrant glycosylation is considered to be a hallmark of colorectal cancer(CRC),as demonstrated by various studies.While the N-glycosylation of cell lines and serum has been widely examined,the analysis of cancer-asso...Aberrant glycosylation is considered to be a hallmark of colorectal cancer(CRC),as demonstrated by various studies.While the N-glycosylation of cell lines and serum has been widely examined,the analysis of cancer-associated N-glycans from tissues has been hampered by the heterogeneity of tumors and the complexity of N-glycan structures.To overcome these obstacles,we present a study using laser capture microdissection that makes it possible to largely deconvolute distinct N-glycomic signatures originating from different regions of heterogeneous tissues including cancerous,stromal,and healthy mucosa cells.N-glycan alditols were analyzed by means of porous graphitized carbon liquid chromatographyelectrospray ionization tandem mass spectrometry,enabling the differentiation and structural characterization of isomeric species.In total,116 N-glycans were identified that showed profound differences in expression among cancer,stroma,and normal mucosa.In comparison with healthy mucosa,the cancer cells showed an increase in a2-6 sialylation and monoantennary N-glycans,as well as a decrease in bisected N-glycans.Moreover,specific sialylated and(sialyl-)LewisA/X antigen-carrying N-glycans were exclusively expressed in cancers.In comparison with cancer,the stroma showed lower levels of oligomannosidic and monoantennary N-glycans,LewisA/X epitopes,and sulfation,as well as increased expression of(core-)fucosylation and a2-3 sialylation.Our study reveals the distinct N-glycomic profiles of different cell types in CRC and control tissues,proving the necessity of their separate analysis for the discovery of cancer-associated glycans.展开更多
Heteroatom doped graphitic porous carbon is highly desirable for electrochemical applications because of its excellent conductivity and high surface area.In this study,highly uniform Co-Ni oxide nanoparticleloaded B,N...Heteroatom doped graphitic porous carbon is highly desirable for electrochemical applications because of its excellent conductivity and high surface area.In this study,highly uniform Co-Ni oxide nanoparticleloaded B,N-doped hierarchical graphitic porous carbon was prepared through a dual pyrolysis process.Graphene dispersed chitosan hydrogel was first used as a precursor to fabricate the porous carbon(GCS–C)at 700℃.Co and Ni oxide nanoparticles were further anchored on the porous carbon through chemical reduction and calcined at high temperature.The structure of the porous carbon was optimized by the introduction of graphene to the chitosan hydrogel.The graphitic degree of the porous carbon was significantly improved by the Co and Ni species.The heteroatom B and N were found to be well doped in the composite.These features enable the composite to be an excellent candidate for supercapacitor electrodes.The composite demonstrates a high capacitance(1266.7 F g-1 at 1 A g-1)and excellent stability.展开更多
The commercialization of the lithium-sulfur(Li-S)batteries is severely hampered by the shuttle effect and sluggish kinetics of lithium polysulfides(Li PSs).In this study,porous tubular graphitic carbon nitride(PTCN)wa...The commercialization of the lithium-sulfur(Li-S)batteries is severely hampered by the shuttle effect and sluggish kinetics of lithium polysulfides(Li PSs).In this study,porous tubular graphitic carbon nitride(PTCN)was synthesized as the sulfur host by hydrothermal treatment,thermal shock and etching methods.By etching technology,the hollow nanotube tentacles grow on the tube wall of PTCN,the mesoporous appears on the inner wall,and a large number of nitrogen defects are introduced.The verticallyrooted hollow nanotube tentacles on the PTCN surface facilitate electron conduction for sulfur redox reactions.The hollow and porous architecture exposes plentiful active interfaces for accelerated redox conversion of polysulfide.Furthermore,the nitrogen defects in PTCN enable more excellent intrinsic conductivity,higher adsorbability and conversion catalytic activity to Li PSs.Based on the above synergetic effect,the batteries with PTCN/S cathodes realize a high discharge capacity of 504 m Ah g^(-1) at 4 C and a stable cycling behavior over 500 cycles with a low capacity decay of 0.063%per cycle.The results indicate a promising approach todesigning a high performance electrode material for Li-S batteries.展开更多
Porous carbon skeletons(PCSs)derived from isocyanate-based aromatic polyimide foams(PIFs)by high-temperature pyrolysis are very promising in the fabrication of high-performance polymer composite foams for electromagne...Porous carbon skeletons(PCSs)derived from isocyanate-based aromatic polyimide foams(PIFs)by high-temperature pyrolysis are very promising in the fabrication of high-performance polymer composite foams for electromagnetic interference(EMI)shielding due to their efficient conductive networks and facile preparation process.However,severe volumetric shrinkage and low graphitization degree is not conducive to enhancing the shielding efficiency of the PCSs.Herein,ferric acetylacetonate and carbon-nanotube coating have been introduced in isocyanate-based PIFs to greatly suppress the serious shrinkage during pyrolysis and improve the graphitization degree of the final carbon foams through the Fe-catalytic graphitization process,thereby endowing them with better EMI-shielding performance even at lower pyrolysis temperature compared to the control samples.Moreover,compressible polydimethylsiloxane(PDMS)composite foams with the as-prepared carbon foams as prefabricated PCSs have also been fabricated,which could provide not only stable shielding effectiveness(SE)performance even after a thousand compressions,but also multiple functions of Joule heating,thermal insulation and infrared stealth.This study offers a feasible route to prepare high-performance PCSs in a more energy-efficient manner via PIF pyrolysis,which is very promising in the manufacture of multifunctional conductive polymer composite foams.展开更多
Creating pores in suprastructures of two-dimensional (2D) materials while controlling the orientation of the 2D building blocks is important in achieving large specific surface areas and tuning the anisotropic prope...Creating pores in suprastructures of two-dimensional (2D) materials while controlling the orientation of the 2D building blocks is important in achieving large specific surface areas and tuning the anisotropic properties of the obtained functional hierarchical structures. In this contribution, we report that arranging graphitic carbon nitride (g-C3N4) nanosheets into one-dimensional (1D) architectures with controlled orientation has been achieved by using 1D oriented melem hydrate fibers as the synthetic precursor via a polycondensation process, during which the removal of water molecules and release of ammonia gas led to the creation of pores without destroying the 1D morphology of the oriented structures. The resulting porous g-C3N4 fibers with both meso- and micro-sized pores and largely exposed edges exhibited good sensing sensitivity and selectivity towards NO2. The sensing performance was further improved by hybridization of the porous fibers with Au nanoparticles (Au NPs), leading to a detection limit of 60 ppb under ambient conditions. Our results suggest that the highly porous g-C3N4 fibers and the related hybrid structures with largely exposed graphitic layer edges are excellent sensing platforms and may also show promise in other electronic and electrochemical applications.展开更多
Constructing 2D/2D face-to-face heterojunctions is believed to be an effective strategy to enhance photocatalytic performance due to the enlarged contact interface and increased surface active sites.Herein,2D porous N...Constructing 2D/2D face-to-face heterojunctions is believed to be an effective strategy to enhance photocatalytic performance due to the enlarged contact interface and increased surface active sites.Herein,2D porous NiCo oxyphosphide(NiCoOP)was synthesized for the first time and coupled with graphitic carbon nitride(g-C_(3)N_(4))nanosheets to form 2D/2D heterojunctions via an in-situ phosphating method.The optimal 4 wt.%2D/2D NiCoOP/g-C_(3)N_(4)(OPCN)photocatalyst achieves a hydrogen evolution rate of 1.4 mmol·h^(−1)·g^(−1),which is 33 times higher than that of pure g-C_(3)N_(4).The greatly improved photocatalytic performance of the composite photocatalysts could be attributed to the formation of interfacial surface bonding states and sufficient charge transfer channels for accelerating carrier separation and transfer and the porous structure of NiCoOP nanosheets with abundant surface active sites for promoting surface reactions.Amazingly,the 2D/2D OPCN composite photocatalysts also exhibit superior stability during photocatalytic reactions.This study not only designs new noble-metal-free NiCoOP/g-C_(3)N_(4)composite photocatalysts but also provides a new sight in fabricating face-to-face 2D/2D heterojunctions for their application in energy conversion areas.展开更多
Photocatalytic nitrogen fixation has been explored as a feasible pathway for ammonia synthesis.How-ever,the convenient and efficient preparation of photocatalysts for nitrogen fixation remains a challenge.Meanwhile,th...Photocatalytic nitrogen fixation has been explored as a feasible pathway for ammonia synthesis.How-ever,the convenient and efficient preparation of photocatalysts for nitrogen fixation remains a challenge.Meanwhile,the reaction pathway and mechanism of photocatalytic nitrogen fixation are unclear.Herein,single-atom Fe-porous g-C_(3)N_(4)(FPx)samples were manufactured using a one-step anneal technique via bubble template and direct metal atomization.Characterization results indicate that FPx has a porous structure and single-atom Fe.The porous structure exposed more active centers.Simultaneously,single-atom Fe changes the adsorption mode of N_(2)from physical to chemical and turns the photocatalytic ni-trogen fixation from the associative distal pathway to the associative alternating pathway.Consequently,without any sacrificial agent or cocatalysts,FPx presents a prominent increase in photocatalytic activ-ity,reaching 62.42μmol h^(−1)g^(−1),over fivefold larger than that of bulk g-C_(3)N_(4).This work provides new insights into photocatalytic nitrogen fixation and achieves efficient N_(2)photoreduction by constructing single-atom photocatalysts.展开更多
Graphitic carbon nitride with nitrogen vacancies(NV-g-C_(3)N_(4))as a photocatalyst has been studied in solardriven energy conversion.However,expensive and rare noble metal co-catalysts such as Pt or Pd are required i...Graphitic carbon nitride with nitrogen vacancies(NV-g-C_(3)N_(4))as a photocatalyst has been studied in solardriven energy conversion.However,expensive and rare noble metal co-catalysts such as Pt or Pd are required in the photocatalytic H_(2)evolution.Consequently,the exploration of low-cost and high-performance co-catalysts to replace expensive and rare noble metals has received more and more attention.Herein,a novel hierarchical porous NiO anchored on NV-g-C_(3)N_(4)is successfully fabricated.The NV-g-C_(3)N_(4)/NiO photocatalysts exhibited outstanding H_(2)evolution rate under visible light irradiation in absence of noble metal cocatalysts.The optimized NV-g-C_(3)N_(4)/NiO(the mass ratio of NiO is*1.7%)achieved a maximum H2 evolution rate of 170.60 lmol·g^(-1)·h^(-1),exhibiting*8.3-fold enhancement as compared to that of NV-g-C3N4.NiO as co-catalyst provided more active sites for photocatalytic H2 evolution.Moreover,on the interface of NV-g-C_(3)N_(4)/NiO,an interface electric field is formed between NiO and host nitrogen-vacated g-C3N4,facilitating the transfer of the photogenerated electrons from NV-g-C_(3)N_(4)to NiO co-catalyst,resulting in significantly promoted migration and separation efficiency of the photogenerated charge carriers.展开更多
Rational design and synthesis of highly efficient and robust photocatalysts with positive exciton splitting and interfacial charge transfer for environmental applications is critical.Herein,aiming at overcoming the co...Rational design and synthesis of highly efficient and robust photocatalysts with positive exciton splitting and interfacial charge transfer for environmental applications is critical.Herein,aiming at overcoming the common shortcomings of traditional photocatalysts such as weak photoresponsivity,rapid combination of photo-generated carriers and unstable structure,a novel Ag-bridged dual Z-scheme g-C_(3)N_(4)/BiOI/AgI plasmonic heterojunction was successfully synthesized using a facile method.Results showed that Ag-AgI nanoparticles and three-dimensional(3D)BiOI microspheres were decorated highly uniformly on the 3D porous g-C_(3)N_(4) nanosheet,resulting in a higher specific surface area and abundant active sites.The optimized 3D porous dual Z-scheme g-C_(3)N_(4)/BiOI/Ag-AgI manifested exceptional photocatalytic degradation efficiency of tetracycline(TC)in water with approximately 91.8%degradation efficiency within 165 min,outperforming majority of the reported g-C_(3)N_(4)-based photocatalysts.Moreover,g-C_(3)N_(4)/BiOI/Ag-AgI exhibited good stability in terms of activity and structure.In-depth radical scavenging and electron paramagnetic resonance(EPR)analyses confirmed the relative contributions of various scavengers.Mechanism analysis indicated that the improved photocatalytic performance and stability were ascribed to the highly ordered 3D porous framework,fast electron transfer of dual Z-scheme heterojunction,desirable photocatalytic performance of BiOI/AgI and synergistic effect of Ag plasmas.Therefore,the 3D porous Z-scheme g-C_(3)N_(4)/BiOI/Ag-AgI heterojunction had a good prospect for applications in water remediation.The current work provides new insight and useful guidance for designing novel structural photocatalysts for environment-related applications.展开更多
Graphitic carbon nitride(g-C_(3)N_(4),denoted as CN)has gained significant attention for its potential applications in treating environmental pollutants due to its unique microstructure and chemical properties.In this...Graphitic carbon nitride(g-C_(3)N_(4),denoted as CN)has gained significant attention for its potential applications in treating environmental pollutants due to its unique microstructure and chemical properties.In this study,porous CN co-doped with Co and Mo(Co/Mo-CN)was successfully synthesized using a convenient thermal polymerization method involving polyoxometalate precursor of(NH_(4))_(4)[Co(Ⅱ)Mo_(6)O_(24)H_(6)](CoMo_(6)).The single-source precursor of CoMo_(6)was not only as a pore forming agent by oxidation etching,but also as a bimetallic doping source.Compared with pristine CN(P-CN),Co/Mo-CN possessed more advantages,such as high specific surface area,plentiful exposed active sites,extending the light absorption capability,rapid separation of photogenerated charge carriers,narrowed bandgap and more negative conduction band potential.As expected,the Co/Mo-CN exhibited a significant enhancement of adsorption ability for cationic dyes and photoreduction Cr(Ⅵ)under visible light irradiation compared to P-CN.This research opened a new pathway designing multifunctional CN-based materials.展开更多
基金the National Natural Science Foundation of China(No.52004179)the Natural Nat-ural Science Foundation of Guangxi Province,China(No.2020GXNSFAA159015)Shanxi Water and Wood New Carbon Materials Technology Co.,Ltd.,China,and Shanxi Wote Haimer New Materials Technology Co.,Ltd,China.
文摘The development of anode materials with high rate capability and long charge-discharge plateau is the key to improve per-formance of lithium-ion capacitors(LICs).Herein,the porous graphitic carbon(PGC-1300)derived from a new triply interpenetrated co-balt metal-organic framework(Co-MOF)was prepared through the facile and robust carbonization at 1300°C and washing by HCl solu-tion.The as-prepared PGC-1300 featured an optimized graphitization degree and porous framework,which not only contributes to high plateau capacity(105.0 mAh·g^(−1)below 0.2 V at 0.05 A·g^(−1)),but also supplies more convenient pathways for ions and increases the rate capability(128.5 mAh·g^(−1)at 3.2 A·g^(−1)).According to the kinetics analyses,it can be found that diffusion regulated surface induced capa-citive process and Li-ions intercalation process are coexisted for lithium-ion storage.Additionally,LIC PGC-1300//AC constructed with pre-lithiated PGC-1300 anode and activated carbon(AC)cathode exhibited an increased energy density of 102.8 Wh·kg^(−1),a power dens-ity of 6017.1 W·kg^(−1),together with the excellent cyclic stability(91.6%retention after 10000 cycles at 1.0 A·g^(−1)).
基金the Science and Technology Research Project of Education Department of Jilin Province(JJKH20220683KJ)Natural Science Foundation of Jilin Province(20220101093JC).
文摘Common strategies for catalytic graphitization of biochar into graphitic porous carbon(GPC)still face great challenges,such as the realization of simple procedures,energy conservation,and green processes.Controlling over the graphitization degree and pore structure of biochar is the key to its structural diversification.Herein,a clean and energy-efficient method is developed to synthesize adjustable graphitic degree and structure porosity GPC from rice husk-based carbon(RHC)at a relatively low temperature of 800–1000°C with environment-benign organometallic catalyst ethylenediaminetetraacetic acid ferric sodium salt(EDTA-iron)and the recovery ratio of catalyst is as high as 97%.The formed by the organic ligands of EDTA-iron facilitates the etching of RHC surface and pore by iron,resulting in highly graphitized and developed porous GPCs.The pore structure and graphitization degree of GPCs can be adjusted by altering the catalyst loading,temperature,and holding time.The catalyst EDTA-iron with a lower concentration mainly plays the role of etching,which promotes the formation of porous carbon with larger surface area(SBET=1187.2 m^(2)·g^(-1)).The catalyst with higher concentration mainly plays the role of catalyzing graphitization and promotes the obtaining of graphitic carbon with high graphitization degree(ID/IG=0.19).The mechanism of EDTA-iron catalyzed graphitization of RHC is explored by the comprehensive analysis of BET,XRD,Raman,TEM and TGA.This research not only provides an efficient method for the preparation of high-quality biomass-based graphite carbon,but also provides a feasible method for the preparation of biomass-based porous carbon.
基金supported by the National Natural Science Foundation of China (grant no. 51672151).
文摘Lithium-ion hybrid supercapacitors(Li-HSCs) and dual-ion batteries(DIBs) are two types of energy storage devices that have attracted extensive research interest in recent years. Li-HSCs and DIBs have similarities in device structure, tendency for ion migration, and energy storage mechanisms at the negative electrode. However, these devices have differences in energy storage mechanisms and working potentials at the positive electrode. Here, we first realize the integration of a Li-HSC and a DIB to form a dual-ion hybrid supercapacitor(DIHSC), by employing mesocarbon microbead(MCMB)-based porous graphitic carbon(PGC) with a partially graphitized structure and porous structure as a positive electrode material. The MCMB-PGC-based DIHSC exhibits a novel dual-ion battery-capacitor hybrid mechanism: it exhibits excellent electronic double-layer capacitor(EDLC) behavior like a Li-HSC in the low-middle wide potential range and anion intercalation/de-intercalation behavior like a DIB in the high-potential range. Two types of mechanisms are observed in the electrochemical characterization process, and the energy density of the new DIHSC is significantly increased.
基金financially supported by the Fundamental Research Funds for the National Natural Science Foundation of China(Nos.21071107,21277094,and21103119)Production and Research Collaborative Innovation Project of Jiangsu Province(No.BY2012123)+9 种基金Natural Science Foundation of Jiangsu Province(No.BK2012167)Scienceand Technology Pillar Program(Industry)of Jiangsu Province(No.BE2012101)Collegiate Natural Science Fund of Jiangsu Province(Nos.12KJA430005,09KJB30003,and11KJB430012)Key Laboratory for Environment Functional Materials of Suzhou(No.SZS201008)A Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD),Applied Basic Research Project of Suzhou(No.SYG201242)Industrial Surport Project of Suzhou(No.SG201138)Jiangsu Key Laboratory of Material Tribology(No.Kjsmcx2011001)Jiangsu Key Laboratory for Photon Manufacturing(No.GZ201111)Jiangsu Provincial Key Laboratory for Interventional Medical Devices(No.Jr1210)Creative Project of Postgraduate of Jiangsu Province(No.CXZZ11_0954)
文摘A hierarchical micro-nano porous carbon material (MNC) was prepared using expanded graphite (EG), sucrose, and phosphoric acid as raw materials, followed by sucrose-phosphoric acid solution impregnation, solidification, carbonization and activation. Nitrogen adsorption and mercury porosimetry show that mixed nanopores and micropores coexist in MNC with a high specific surface area of 1978 m2·g-1 and a total pore volume of 0.99 cm3·g-1. In addition, the MNC is found to consist of EG and activated carbon with the latter deposited on the interior and the exterior surfaces of the EG pores. The thickness of the activated carbon layer is calculated to be about one hundred nanometers and is further confirmed by scanning electron microscope (SEM) and transmission election microscope (TEM). A maximum static phenol adsorption of 241.2 mg·g-1 was obtained by using MNC, slightly higher than that of 220.4 mg·g-1 by using commercial activated carbon (CAC). The phenol adsorption kinetics were investigated and the data fitted well to a pseudo-second-order model. Also, an intra-particle diffusion mechanism was proposed. Furthermore, it is found that the dynamic adsorption capacity of MNC is nearly three times that of CAC. The results suggest that the MNC is a more efficient adsorbent than CAC for the removal of phenol from aqueous solution.
文摘The active site amount of photocatalysts,being the key factors in photocatalytic reactions,directly affects the photocatalytic performance of the photocatalyst.Pristine graphitic carbon nitride(g‐C_(3)N_(4))exhibits moderate photocatalytic activity due to insufficient active sites.In this study,cyano‐modified porous g‐C_(3)N_(4)nanosheets(MCN‐0.5)were synthesized through molecular self‐assembly and alkali‐assisted strategies.The cyano group acted as the active site of the photocatalytic reaction,because the good electron‐withdrawing property of the cyano group promoted carrier separation.Benefiting from the effect of the active sites,MCN‐0.5 exhibited significantly enhanced photocatalytic activity for CO2 reduction under visible light irradiation.Notably,the photocatalytic activity of MCN‐0.5 was significantly reduced when the cyano groups were removed by hydrochloric acid(HCl)treatment,further verifying the role of cyano groups as active sites.The photoreduction of Pt nanoparticles provided an intuitive indication that the introduction of cyano groups provided more active sites for the photocatalytic reaction.Furthermore,the controlled experiments showed that g‐C_(3)N_(4)grafted with cyano groups using melamine as the precursor exhibited enhanced photocatalytic activity,which proved the versatility of the strategy for enhancing the activity of g‐C_(3)N_(4)via cyano group modification.In situ diffuse reflectance infrared Fourier transform spectroscopy and theoretical calculations were used to investigate the mechanism of enhanced photocatalytic activity for CO2 reduction by cyano‐modified g‐C_(3)N_(4).This work provides a promising route for promoting efficient solar energy conversion by designing active sites in photocatalysts.
基金supported by the National Natural Science Foundation of China(51568049,51208248,51468043,21366024)the National Science Fund for Excellent Young Scholars(51422807)+1 种基金the Natural Science Foundation of Jiangxi Province,China(20161BAB206118,20114BAB213015)the Natural Science Foundation of Jiangxi Provincial Department of Education,China(GJJ14515,GJJ12456)~~
文摘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.
基金supported by the National Natural Science Foundation of China (51568049, 51208248, 51468043, 21366024)the National Science Fund for Excellent Young Scholars (51422807)+1 种基金the Natural Science Foundation of Jiangxi Province, China (20161BAB206118, 20114BAB213015)the Natural Science Foundation of Jiangxi Provincial Department of Education, China (GJJ14515, GJJ12456)~~
文摘A series of highly dispersed platinum‐deposited porous g‐C3N4 (Pt/pg‐C3N4) were successfully fabricated by a simple in situ photoreduction strategy using chloroplatinic acid and porous g‐C3N4 as precursors. Porous g‐C3N4 was fabricated by a pretreatment strategy using melamine as a raw material.The morphology, porosity, phase, chemical structure, and optical and electronic properties ofas‐prepared Pt/pg‐C3N4 were characterized. The photocatalytic activity of as‐prepared Pt/pg‐C3N4was preliminarily evaluated by the degradation of aqueous azo dyes methyl orange under visible light irradiation. The as‐prepared Pt/pg‐C3N4 were further applied to the degradation and mineralization of aqueous 4‐fluorophenol. The recyclability of Pt/pg‐C3N4 was evaluated under four consecutive photocatalytic runs.
基金the National Natural Science Foundation of China(No.51804344)the Program of Huxiang Young Talents(No.2019RS2002)+1 种基金the Innovation and Entrepreneurship Project of Hunan Province,China(No.2018GK5026)the Innovation-Driven Project of Central South University(No.2020CX027)。
文摘Graphitic carbons with reasonable pore volume and appropriate graphitization degree can provide efficient Li+/electrolyte-transfer channels and ameliorate the sluggish dynamic behavior of battery-type carbon negative electrode in lithium-ion capacitors(LICs).In this work,onion-like graphitic carbon materials are obtained by using carbon quantum dots as precursors after sintering,and the effects of alkali metal salts on the structure,morphology and performance of the samples are focused.The results show that alkali metal salts as activator can etch graphitic carbons,and the specific surface area and pore size distribution are intimately related to the description of the alkali metal salt.Moreover,it also affects the graphitization degree of the materials.The porous graphitic carbons(SGCs)obtained by NaCl activation exhibit high specific surface area(77.14 m^(2)·g^(-1))and appropriate graphitization degree.It is expectable that the electrochemical performance for lithium-ions storage can be largely promoted by the smart combination of catalytic graphitization and pores-creating strategy.High-performance LICs(S-GCs//AC LICs)are achieved with high energy density of 92 Wh·kg^(-1)and superior rate capability(66.3 Wh·kg^(-1)at10 A·g^(-1))together with the power density as high as10020.2 W·kg^(-1).
文摘Aberrant glycosylation is considered to be a hallmark of colorectal cancer(CRC),as demonstrated by various studies.While the N-glycosylation of cell lines and serum has been widely examined,the analysis of cancer-associated N-glycans from tissues has been hampered by the heterogeneity of tumors and the complexity of N-glycan structures.To overcome these obstacles,we present a study using laser capture microdissection that makes it possible to largely deconvolute distinct N-glycomic signatures originating from different regions of heterogeneous tissues including cancerous,stromal,and healthy mucosa cells.N-glycan alditols were analyzed by means of porous graphitized carbon liquid chromatographyelectrospray ionization tandem mass spectrometry,enabling the differentiation and structural characterization of isomeric species.In total,116 N-glycans were identified that showed profound differences in expression among cancer,stroma,and normal mucosa.In comparison with healthy mucosa,the cancer cells showed an increase in a2-6 sialylation and monoantennary N-glycans,as well as a decrease in bisected N-glycans.Moreover,specific sialylated and(sialyl-)LewisA/X antigen-carrying N-glycans were exclusively expressed in cancers.In comparison with cancer,the stroma showed lower levels of oligomannosidic and monoantennary N-glycans,LewisA/X epitopes,and sulfation,as well as increased expression of(core-)fucosylation and a2-3 sialylation.Our study reveals the distinct N-glycomic profiles of different cell types in CRC and control tissues,proving the necessity of their separate analysis for the discovery of cancer-associated glycans.
基金the financial support from the National Natural Science Foundation of China(Nos.51861005 and 51861004)the Innovation Project of GUET Graduate Education(2019YCXS113)+1 种基金the GUET Excellent Graduate Thesis Program(17YJPYSS32)the Guangxi Natural Science Foundation(2017AD23029).
文摘Heteroatom doped graphitic porous carbon is highly desirable for electrochemical applications because of its excellent conductivity and high surface area.In this study,highly uniform Co-Ni oxide nanoparticleloaded B,N-doped hierarchical graphitic porous carbon was prepared through a dual pyrolysis process.Graphene dispersed chitosan hydrogel was first used as a precursor to fabricate the porous carbon(GCS–C)at 700℃.Co and Ni oxide nanoparticles were further anchored on the porous carbon through chemical reduction and calcined at high temperature.The structure of the porous carbon was optimized by the introduction of graphene to the chitosan hydrogel.The graphitic degree of the porous carbon was significantly improved by the Co and Ni species.The heteroatom B and N were found to be well doped in the composite.These features enable the composite to be an excellent candidate for supercapacitor electrodes.The composite demonstrates a high capacitance(1266.7 F g-1 at 1 A g-1)and excellent stability.
基金Natural Science Foundation of Hebei Province of China(Nos.B2020202052B2021202028)+6 种基金Outstanding Youth Project of Guangdong Natural Science Foundation(No.2021B1515020051)the Program for the Outstanding Young Talents of Hebei Province,China(YG.Z.)Chunhui Project of Ministry of Education of the People’s Republic of China(No.Z2017010)Department of Science and Technology of Guangdong Province(No.2020B0909030004)Guangdong Innovative and Entrepreneurial Team Program(No.2016ZT06C517)Science and Technology Program of Guangzhou(No.2019050001)Science and Technology Program of Zhaoqing(No.2019K038)。
文摘The commercialization of the lithium-sulfur(Li-S)batteries is severely hampered by the shuttle effect and sluggish kinetics of lithium polysulfides(Li PSs).In this study,porous tubular graphitic carbon nitride(PTCN)was synthesized as the sulfur host by hydrothermal treatment,thermal shock and etching methods.By etching technology,the hollow nanotube tentacles grow on the tube wall of PTCN,the mesoporous appears on the inner wall,and a large number of nitrogen defects are introduced.The verticallyrooted hollow nanotube tentacles on the PTCN surface facilitate electron conduction for sulfur redox reactions.The hollow and porous architecture exposes plentiful active interfaces for accelerated redox conversion of polysulfide.Furthermore,the nitrogen defects in PTCN enable more excellent intrinsic conductivity,higher adsorbability and conversion catalytic activity to Li PSs.Based on the above synergetic effect,the batteries with PTCN/S cathodes realize a high discharge capacity of 504 m Ah g^(-1) at 4 C and a stable cycling behavior over 500 cycles with a low capacity decay of 0.063%per cycle.The results indicate a promising approach todesigning a high performance electrode material for Li-S batteries.
基金Youth Innovation Promotion Association of Chinese Academy of Sciences(No.2022300)Natural Science Foundation of Ningbo(No.202003N4026)China Postdoctoral Science Foundation(No.2020M682375)’Key Scientific Research Projects of Colleges and Universities in Henan Province(No.21A430025).
文摘Porous carbon skeletons(PCSs)derived from isocyanate-based aromatic polyimide foams(PIFs)by high-temperature pyrolysis are very promising in the fabrication of high-performance polymer composite foams for electromagnetic interference(EMI)shielding due to their efficient conductive networks and facile preparation process.However,severe volumetric shrinkage and low graphitization degree is not conducive to enhancing the shielding efficiency of the PCSs.Herein,ferric acetylacetonate and carbon-nanotube coating have been introduced in isocyanate-based PIFs to greatly suppress the serious shrinkage during pyrolysis and improve the graphitization degree of the final carbon foams through the Fe-catalytic graphitization process,thereby endowing them with better EMI-shielding performance even at lower pyrolysis temperature compared to the control samples.Moreover,compressible polydimethylsiloxane(PDMS)composite foams with the as-prepared carbon foams as prefabricated PCSs have also been fabricated,which could provide not only stable shielding effectiveness(SE)performance even after a thousand compressions,but also multiple functions of Joule heating,thermal insulation and infrared stealth.This study offers a feasible route to prepare high-performance PCSs in a more energy-efficient manner via PIF pyrolysis,which is very promising in the manufacture of multifunctional conductive polymer composite foams.
文摘Creating pores in suprastructures of two-dimensional (2D) materials while controlling the orientation of the 2D building blocks is important in achieving large specific surface areas and tuning the anisotropic properties of the obtained functional hierarchical structures. In this contribution, we report that arranging graphitic carbon nitride (g-C3N4) nanosheets into one-dimensional (1D) architectures with controlled orientation has been achieved by using 1D oriented melem hydrate fibers as the synthetic precursor via a polycondensation process, during which the removal of water molecules and release of ammonia gas led to the creation of pores without destroying the 1D morphology of the oriented structures. The resulting porous g-C3N4 fibers with both meso- and micro-sized pores and largely exposed edges exhibited good sensing sensitivity and selectivity towards NO2. The sensing performance was further improved by hybridization of the porous fibers with Au nanoparticles (Au NPs), leading to a detection limit of 60 ppb under ambient conditions. Our results suggest that the highly porous g-C3N4 fibers and the related hybrid structures with largely exposed graphitic layer edges are excellent sensing platforms and may also show promise in other electronic and electrochemical applications.
基金the National Natural Science Foundation of China(Nos.52072197 and 52102272)Taishan Scholar Young Talent Program(No.tsqn201909114)+5 种基金the Natural Science Foundation of Shandong Province(No.ZR2021QE063)Youth Innovation and Technology Foundation of Shandong Higher Education Institutions,China(No.2019KJC004)Major Scientific and Technological Innovation Project(No.2019JZZY020405)Outstanding Youth Foundation of Shandong Province,China(No.ZR2019JQ14)Major Basic Research Program of the Natural Science Foundation of Shandong Province(No.ZR2020ZD09)Talent Foundation funded by Province and Ministry Co-construction Collaborative Innovation Center of Eco-chemical Engineering(No.STHGYX2213).
文摘Constructing 2D/2D face-to-face heterojunctions is believed to be an effective strategy to enhance photocatalytic performance due to the enlarged contact interface and increased surface active sites.Herein,2D porous NiCo oxyphosphide(NiCoOP)was synthesized for the first time and coupled with graphitic carbon nitride(g-C_(3)N_(4))nanosheets to form 2D/2D heterojunctions via an in-situ phosphating method.The optimal 4 wt.%2D/2D NiCoOP/g-C_(3)N_(4)(OPCN)photocatalyst achieves a hydrogen evolution rate of 1.4 mmol·h^(−1)·g^(−1),which is 33 times higher than that of pure g-C_(3)N_(4).The greatly improved photocatalytic performance of the composite photocatalysts could be attributed to the formation of interfacial surface bonding states and sufficient charge transfer channels for accelerating carrier separation and transfer and the porous structure of NiCoOP nanosheets with abundant surface active sites for promoting surface reactions.Amazingly,the 2D/2D OPCN composite photocatalysts also exhibit superior stability during photocatalytic reactions.This study not only designs new noble-metal-free NiCoOP/g-C_(3)N_(4)composite photocatalysts but also provides a new sight in fabricating face-to-face 2D/2D heterojunctions for their application in energy conversion areas.
基金supported by the Jiangxi Provincial Natural Science Foundation(No.20224BAB213016)Jiangxi Province tech-nology innovation guidance project(grant No.20212BDH81036)Science and Technology Project of the Education Department of Jiangxi Province(No.GJJ200457).
文摘Photocatalytic nitrogen fixation has been explored as a feasible pathway for ammonia synthesis.How-ever,the convenient and efficient preparation of photocatalysts for nitrogen fixation remains a challenge.Meanwhile,the reaction pathway and mechanism of photocatalytic nitrogen fixation are unclear.Herein,single-atom Fe-porous g-C_(3)N_(4)(FPx)samples were manufactured using a one-step anneal technique via bubble template and direct metal atomization.Characterization results indicate that FPx has a porous structure and single-atom Fe.The porous structure exposed more active centers.Simultaneously,single-atom Fe changes the adsorption mode of N_(2)from physical to chemical and turns the photocatalytic ni-trogen fixation from the associative distal pathway to the associative alternating pathway.Consequently,without any sacrificial agent or cocatalysts,FPx presents a prominent increase in photocatalytic activ-ity,reaching 62.42μmol h^(−1)g^(−1),over fivefold larger than that of bulk g-C_(3)N_(4).This work provides new insights into photocatalytic nitrogen fixation and achieves efficient N_(2)photoreduction by constructing single-atom photocatalysts.
基金This study was financially supported by the National Natural Science Foundation of China(Nos.22075072 and 52003079)Hubei Provincial Natural Science Foundation of China(No.2019CFB568).
文摘Graphitic carbon nitride with nitrogen vacancies(NV-g-C_(3)N_(4))as a photocatalyst has been studied in solardriven energy conversion.However,expensive and rare noble metal co-catalysts such as Pt or Pd are required in the photocatalytic H_(2)evolution.Consequently,the exploration of low-cost and high-performance co-catalysts to replace expensive and rare noble metals has received more and more attention.Herein,a novel hierarchical porous NiO anchored on NV-g-C_(3)N_(4)is successfully fabricated.The NV-g-C_(3)N_(4)/NiO photocatalysts exhibited outstanding H_(2)evolution rate under visible light irradiation in absence of noble metal cocatalysts.The optimized NV-g-C_(3)N_(4)/NiO(the mass ratio of NiO is*1.7%)achieved a maximum H2 evolution rate of 170.60 lmol·g^(-1)·h^(-1),exhibiting*8.3-fold enhancement as compared to that of NV-g-C3N4.NiO as co-catalyst provided more active sites for photocatalytic H2 evolution.Moreover,on the interface of NV-g-C_(3)N_(4)/NiO,an interface electric field is formed between NiO and host nitrogen-vacated g-C3N4,facilitating the transfer of the photogenerated electrons from NV-g-C_(3)N_(4)to NiO co-catalyst,resulting in significantly promoted migration and separation efficiency of the photogenerated charge carriers.
基金supported by the National Natural Science Foundation of China(Nos.22106020 and 42122056)the KeyArea Research and Development Program of Guangdong Province(No.2020B1111350002)+1 种基金the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(No.2017BT01Z032)the Guangdong Basic and Applied Basic Research Foundation(No.2020A1515110718).
文摘Rational design and synthesis of highly efficient and robust photocatalysts with positive exciton splitting and interfacial charge transfer for environmental applications is critical.Herein,aiming at overcoming the common shortcomings of traditional photocatalysts such as weak photoresponsivity,rapid combination of photo-generated carriers and unstable structure,a novel Ag-bridged dual Z-scheme g-C_(3)N_(4)/BiOI/AgI plasmonic heterojunction was successfully synthesized using a facile method.Results showed that Ag-AgI nanoparticles and three-dimensional(3D)BiOI microspheres were decorated highly uniformly on the 3D porous g-C_(3)N_(4) nanosheet,resulting in a higher specific surface area and abundant active sites.The optimized 3D porous dual Z-scheme g-C_(3)N_(4)/BiOI/Ag-AgI manifested exceptional photocatalytic degradation efficiency of tetracycline(TC)in water with approximately 91.8%degradation efficiency within 165 min,outperforming majority of the reported g-C_(3)N_(4)-based photocatalysts.Moreover,g-C_(3)N_(4)/BiOI/Ag-AgI exhibited good stability in terms of activity and structure.In-depth radical scavenging and electron paramagnetic resonance(EPR)analyses confirmed the relative contributions of various scavengers.Mechanism analysis indicated that the improved photocatalytic performance and stability were ascribed to the highly ordered 3D porous framework,fast electron transfer of dual Z-scheme heterojunction,desirable photocatalytic performance of BiOI/AgI and synergistic effect of Ag plasmas.Therefore,the 3D porous Z-scheme g-C_(3)N_(4)/BiOI/Ag-AgI heterojunction had a good prospect for applications in water remediation.The current work provides new insight and useful guidance for designing novel structural photocatalysts for environment-related applications.
基金supported by Science and Technology Development Project of Jilin Province(YDZJ202301ZYTS313)Doctoral Research Initiation Fund Project of Jilin Engineering(BSKJ201918)
文摘Graphitic carbon nitride(g-C_(3)N_(4),denoted as CN)has gained significant attention for its potential applications in treating environmental pollutants due to its unique microstructure and chemical properties.In this study,porous CN co-doped with Co and Mo(Co/Mo-CN)was successfully synthesized using a convenient thermal polymerization method involving polyoxometalate precursor of(NH_(4))_(4)[Co(Ⅱ)Mo_(6)O_(24)H_(6)](CoMo_(6)).The single-source precursor of CoMo_(6)was not only as a pore forming agent by oxidation etching,but also as a bimetallic doping source.Compared with pristine CN(P-CN),Co/Mo-CN possessed more advantages,such as high specific surface area,plentiful exposed active sites,extending the light absorption capability,rapid separation of photogenerated charge carriers,narrowed bandgap and more negative conduction band potential.As expected,the Co/Mo-CN exhibited a significant enhancement of adsorption ability for cationic dyes and photoreduction Cr(Ⅵ)under visible light irradiation compared to P-CN.This research opened a new pathway designing multifunctional CN-based materials.