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Journal of Environmental Sciences 2024年第5期139卷 12-22页

作者： Yi Yuan Wen-Long Wang Zhi-Wei Wang Jin Wang Qian-Yuan Wu Key Laboratory of Microorganism Application and Risk Control of Shenzhen Guangdong Provincial Engineering Research Center for Urban Water Recycling and Environmental SafetyInstitute of Environment and EcologyShenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055China Shenzhen Environmental Science and New Energy Technology Engineering Laboratory Tsinghua-Berkeley Shenzhen InstituteShenzhen 518055China College of Materials Science and Engineering Shenzhen UniversityShenzhen 518071China

carbon nitride has been extensively used as a visible-light photocatalyst,but it has the disadvantages of a low specific surface area,rapid electron-hole recombination,and relatively low light absorbance.In this study,single-atom Ag was successfully anchored on ultrathin carbon nitride(UTCN)via thermal polymerization,the catalyst obtained is called AgUTCN.The Ag hardly changed the carbon nitride's layered and porous physical *** exhibited efficient visible-light photocatalytic performances in the degradation of various recalcitrant pollutants,eliminations of 85% were achieved by visible-light irradiation for 1hr.Doping with Ag improved the photocatalytic performance of UTCN by narrowing the forbidden band gap from 2.49 to 2.36 e V and suppressing electron-hole pair recombination.In addition,Ag doping facilitated O_(2) adsorption on UTCN by decreasing the adsorption energy from -0.2 to -2.22 e V and favored the formation of O_(2)^(·-).Electron spin resonance and radical-quenching experiments showed that O_(2)^(·-)was the major reactive species in the degradation of Acetaminophen(paracetamol,APAP).

关键词： Ag single atom carbon nitride Photocatalysis Visible light Adsorption energy Reactive species

Construction of electron rich Fe active sites by FeCu alloy anchoring on carbon nitride for photocatalytic nitrogen reduction

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Rare Metals 2024年第4期43卷 1570-1579页

作者： Gang Dong Cong Huang Fei-Yang Chen Xue-Qin Liu Zhen Li Xiao-Li Su Tao Zeng Yun-Xia Chen Yi-Huang Chen Yang Wang School of Materials Science and Engineering Jingdezhen Ceramic University Faculty of Materials Science and Chemistry China University of Geosciences College of Chemistry and Materials Engineering Wenzhou University

Given the clean and inexhaustible solar energy from solar light,photocatalytic ammonia synthesis is extremely appealing.However,high electron-hole recombination rates and insufficient active sites severely limited N2 photoreaction reduction.Herein,we designed and fabricated FeCu alloy nanoparticles anchored on carbon nitride nanosheets with excellent photocatalyt ic ammonia synthesis performance.As a coupler between Fe and carbon nitride,Cu promotes the separation of photogenerated charge carriers in carbon nitride under solar light irradiation,and renters the semiconductor a forceful electron donor for the Fe active sites.The accumulated electrons at Fe sites furtherly facilitated the adsorption and activation of the molecular nitrogen.Besides,the uniform dispersed FeCu alloy nanoparticles were on carbon nitride nanosheets enhanced the stability of photocataly tic nitrogen reduction reaction,making the artificial photocataly tic ammonia synthesis more sustainable for application.This work highlights that a direct electron transfer channel can be used to regulate the photochemical nitrogen fixation network.

关键词： Photocatalytic N 2 fixation carbon nitride FeCu alloy Active sites Hydrogenation pathway

Advances in Polymeric carbon nitride Photocatalysts for Enhanced CO_(2)Reduction

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China Petroleum Processing & Petrochemical Technology 2024年第2期26卷 1-12页

作者： Liu Bing Sun Shangcong Song Ye Peng Bo Lin Wei SINOPEC Research Institute of Petroleum Processing Co. Ltd.Beijing100083China

Photocatalysis has emerged as a promising alternative for converting and utilizing CO_(2).Polymeric carbon nitride(PCN),typically synthesized through the one-step thermal polycondensation of nitrogen-rich precursors,has shown considerable promise due to its adjustable band structure and inherent safety.Over the past five years,significant literature in this field has identified five primary methods for modifying PCN:morphology modulation,element doping,defect induction,co-catalyst loading,and heterojunction construction.A detailed discussion on how each modification method influences light absorption,charge separation,and surface reaction efficiencies in photocatalysis is provided.Based on these findings,several future directions for the development of PCN-based materials are proposed,such as designing tailored PCN structures for specific photocatalytic reactions and using theoretical calculations to verify and correct results from current characterization methods.Despite the challenges associated with the large-scale synthesis of PCN materials with controllable structures and satisfactory performance,this work offers valuable insights for advancing photocatalytic PCN-based systems for large-scale solar fuel production.

关键词： carbon nitride photocatalysis CO_(2)reduction modification

carbon-nitride-Based Materials for Advanced Lithium-Sulfur Batteries

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Nano-Micro Letters 2022年第12期14卷 579-601页

作者： Wenhao Sun Zihao Song Zhenxing Feng Yaqin Huang Zhichuan J.Xu Yi-Chun Lu Qingli Zou State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China Electrochemical Energy and Interfaces Laboratory Department of Mechanical and Automation EngineeringThe Chinese University of Hong KongHong Kong Special Administrative Region 999077People’s Republic of China School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798Republic of Singapore School of Chemical Biologicaland Environmental EngineeringOregon State UniversityCorvallisOR 97331USA

Lithium-sulfur(Li-S)batteries are promising candidates for next-generation energy storage systems owing to their high energy density and low cost.However,critical challenges including severe shuttling of lithium polysulfides(LiPSs)and sluggish redox kinetics limit the practical application of Li-S batteries.carbon nitrides(C_(x)N_(y)),represented by graphitic carbon nitride(g-C_(3)N_(4)),provide new opportunities for overcoming these challenges.With a graphene-like structure and high pyridinic-N content,g-C_(3)N_(4) can effectively immobilize LiPSs and enhance the redox kinetics of S species.In addition,its structure and properties including electronic conductivity and catalytic activity can be regulated by simple methods that facilitate its application in Li-S batteries.Here,the recent progress of applying C_(x)N_(y)-based materials including the optimized g-C_(3)N_(4),g-C_(3)N_(4)-based composites,and other novel C_(x)N_(y) materials is systematically reviewed in Li-S batteries,with a focus on the structure-activity relationship.The limitations of existing C_(x)N_(y)-based materials are identified,and the perspectives on the rational design of advanced C_(x)N_(y)-based materials are provided for high-performance Li-S batteries.

关键词： Lithium-sulfur batteries carbon nitride Polysulfide conversion Shuttle effect Anode protection

carbon nitride Quantum Dots:A Novel Fluorescent Probe for Non-Enzymatic Hydrogen Peroxide and Mercury Detection

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Journal of Ocean University of China 2023年第6期22卷 1572-1582页

作者： CHEN Lei LI Quan WANG Xing WANG Wentai WANG Lisha Key Laboratory of Marine Chemistry Theory and Technology Ministry of EducationCollege of Chemistry and Chemical EngineeringOcean University of ChinaQingdao 266100China

The mercury species in the ocean(MeHg,Hg^(2+))will be enriched in marine organisms and threaten human health through the food chain.While the excessive H_(2)O_(2)in the metabolic process will produce hydroxyl radicals and accelerate the aging of human cells,causing a series of diseases.Hence,the cost-effective and rapid detection of mercury and H_(2)O_(2)is of urgent requirement and significance.Here,we synthesized emerging graphitic carbon nitride quantum dots(g-CNQDs)with high fluorescence quantum yield(FLQY)of 42.69%via a bottom-up strategy by a facile one-step hydrothermal method.The g-CNQDs can detect the H_(2)O_(2)and Hg^(2+)through the fluorescence quenching effect between g-CNQDs and detected substances.With the presence of KI,g-CNQDs show concentration-dependent fluorescence toward H_(2)O_(2),with a wide detection range of 1–1000μmolL^(-1)and a low detection limit of 0.23μmolL^(-1).The g-CNQDs also show sensitivity toward Hg^(2+)with a detection range of 0–0.1μmolL^(-1)and a detection limit of 0.038μmolL^(-1).This dual-function detection of g-CNQDs has better practical application capability compared to other quantum dot detection.This study may provide a new strategy for g-CNQDs preparation and construct a fluorescence probe that can be used in various systems involving H_(2)O_(2)and Hg^(2+),providing better support for future bifunctional or multifunction studies.

关键词： carbon nitride quantum dots hydrogen peroxide Hg2+ fluorescence probe

Mitigating phytotoxicity of tetracycline by metal-free 8-hydroxyquinoline functionalized carbon nitride photocatalyst

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Journal of Environmental Sciences 2023年第3期125卷 37-46页

作者： Toshali Bhoyar Devthade Vidyasagar Suresh S.Umare Materials and Catalysis Laboratory Department of ChemistryVisvesvaraya National Institute of Technology(VNIT)Nagpur 440010India School of Material Science and Engineering Kyungpook National UniversityDaegu 41566Korea

Photooxidative removal of pharmaceuticals and organic dyes is an effective way to eliminate growing micropollutants. However, photooxidation often results in byproducts as secondary hazardous substances such as phytotoxins. Herein, we found that photooxidation of common antibiotic tetracycline hydrochloride(TCH) over a metal-free 8-hydroxyquinoline(8-HQ) functionalized carbon nitride(CN) photocatalyst significantly reduces the TCH phytotoxic effect. The phytotoxicity test of photocatalytic treated TCH-solution evaluated towards seed growth of Cicer arietinum plant model endowed natural root and shoot growth.This study highlights the conceptual insights in designing of metal-free photocatalyst for environmental remediation.

关键词： carbon nitride 8-Hydroxyquinoline Tetracycline hydrochloride Photocatalyst Phytotoxicity Cicer arietinum

Graphitic carbon nitride loaded with bismuth nanoparticles displays antibacterial photocatalytic activity

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Rare Metals 2022年第5期41卷 1570-1582页

作者： Hui Zhang Ling Li Qian-Qian Li Tao Ma Jia-Qi Gao Jin-Bo Xue Shuang Gao Department of Plastic Surgery Second Hospital of Shanxi Medical UniversityTaiyuan 030001China Key Laboratory of Interface Science and Engineering in Advanced Materials Taiyuan University of TechnologyMinistry of EducationTaiyuan 030024China Department of Materials and Earth Sciences Technical University of DarmstadtDarmstadt 64287Germany

Metal-free graphitic carbon nitride nanomaterials have been widely applied in the medical antibacterial field owing to their high anisotropy, excellent stability,satisfactory biocompatibility, and non-toxicity. Herein, Bi/C_(3)N_(4) nanocomposites were successfully constructed by hydrothermal method followed by loading bismuth on the surface of graphite carbon nitride. Bi nanospheres were tightly combined with the layered g-C_(3)N_(4) surface to promote effective separation of photo-induced charges, which results in the Bi/C_(3)N_(4) composite material that exhibited excellent photocatalytic activity under visible light. In addition, the surface plasmon resonance characteristics of semi-metal Bi further enhanced the visible-light absorption of the Bi/C_(3)N_(4). However, excessive Bi may inhibit the light-trapping ability of Bi/C_(3)N_(4).1.0% Bi/C_(3)N_(4) demonstrates excellent bactericidal efficiency as high as 96.4% against Escherichia coli(E. coli), which is attributed to the promotion of the production of reactive oxidative species.The enhanced mechanism of Bi/C_(3)N_(4) synergistically achieving enhanced photocatalytic antibacterial activity under the coupling of multiple advantages was clarified,providing theoretical guidance for its application in the field of water disinfection and antibacterial treatment.

关键词： carbon nitride Bi nanospheres Schottky barrier ROS Photocatalytic antibacterial

van der Waals type II carbon nitride homojunctions for visible light photocatalytic hydrogen evolution

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Nano Research 2023年第4期16卷 5864-5872页

作者： Xiaojie Li Panpan Zhang Huayang Zhang Wenjie Tian Yangyang Yang Kunsheng Hu Dechao Chen Qin Li Xiaoguang Duan Hongqi Sun Shaobin Wang School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSA 5005Australia Department of Chemical Engineering Curtin UniversityGPO Box U1987PerthWA 6845Australia Queensland Micro-and Nanotechnology Centre School of Engineering and Built EnvironmentGriffith UniversityNathanQLD 4111Australia School of Engineering Edith Cowan UniversityJoondalupWA 6027Australia

Photocatalytic hydrogen evolution reaction(PC-HER)provides a solution to energy crisis and environmental pollution.Herein,different graphitic carbon nitride(g-C_(3)N_(4))-based van der Waals(vdW)type II homojunctions have been fabricated and g-C_(3)N_(4)/Kdoped g-C_(3)N_(4)nanosheets have an outstanding PC-HER rate of 1,243μmol·h^(−1)·g^(−1)under visible light,higher than that of bulk g-C_(3)N_(4),doped g-C_(3)N_(4)nanosheets,and mixed nanosheets.The enhanced PC-HER performance can be ascribed to the cooperative effects of the shortened bandgap,enlarged specific surface area,matched type II energy band structure,“face to face”vdW charge interaction,and peculiarly partite positions of the conduction and valence bands in different layers.Besides,the type II junctions were found superior to binary type II junction.This study highlights the synergistic effect of different strategies in improving the PC-HER capacities of g-C_(3)N_(4),especially the application of particular vdW junctions,and provides new insights to the structures and mechanism.

关键词： van der Waals junction type II junction hydrogen evolution carbon nitride photocatalyst

Aromatic alcohols oxidation and hydrogen evolution over π-electron conjugated porous carbon nitride rods

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Nano Research 2022年第12期15卷 10148-10157页

作者： Jiawei Xia Neeta Karjule Gabriel Mark Michael Volokh Haiqun Chen Menny Shalom Key Laboratory of Advanced Catalytic Materials and Technology Advanced Catalysis and Green Manufacturing Collaborative Innovation CenterChangzhou UniversityChangzhou213164China Department of Chemistry and Ilse Katz Institute for Nanoscale Science and Technology Ben-Gurion University of the NegevBeer-Sheva8410501Israel

Photocatalysis using polymeric carbon nitride(CN)materials is a constantly evolving field,where the variation of synthetic procedures allows the constant improvement of activity by tackling the intrinsic limitations of these materials(optical absorbance,specific surface area,charge migration,etc.).Amongst the possible photocatalytic reactions,the most popular application of CNs is the hydrogen evolution reaction(HER)from water.In this work,we design precisely-controlled carbon-doped porous CN rods with extended π-electron conjugation from supramolecular assemblies of melem and co-monomers,which partially substitute nitrogen for carbon atoms at the pyrimidine ring of the melem.Dense hydrogen bonds and good thermal stability of the melem-based supramolecular framework allow synthesizing a more ordered structure for improved charge migration;the control from the molecular level over the position of carbon-substituted nitrogen positions tailors the band alignment and photogenerated charge separation.The optimal photocatalyst shows an excellent HER rate(up to 10.16 mmol·h-1·g-1 under 100 W white light-emitting diode(LED)irradiation,with an apparent quantum efficiency of 20.0%at 405 nm,which is 23.2 times higher compared to a reference bulk CN).To fully harness the benefits of the developed metal-free CNs,selective oxidation reaction of aromatic alcohols is demonstrated with high conversion and selectivity.

关键词： supramolecular assembly π-electron conjugation carbon nitride photocatalytic hydrogen evolution reaction selective aromatic alcohol oxidation

Homojunction and ohmic contact coexisting carbon nitride for efficient photocatalytic hydrogen evolution

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Nano Research 2023年第7期16卷 8782-8792页

作者： Xiao Fang Lu Chen Hongrui Cheng Xiaoqiong Bian Wenhao Sun Kaining Ding Xinghe Xia Xin Chen Jiefang Zhu Yuanhui Zheng College of Chemistry Fujian Provincial Key Laboratory of Advanced Inorganic Oxygenated MaterialsFuzhou UniversityFuzhou 350116China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350116China College of Physics and Information Engineering Fuzhou UniversityFuzhou 350116China Department of Chemistry−Ångström Laboratory Uppsala UniversityUppsala SE-75121Sweden The Key Laboratory for Ultrafine Materials of The Ministry of Education East China University of Science and TechnologyShanghai 200237China

carbon nitride(CN)has attracted intensive attention as a visible light photocatalyst,but the rapid recombination of photogenerated charge carriers limits its photocatalytic activity.Herein,we develop a new strategy to construct both homojunction and ohmic junction into CN via selectively introducing metallized CN(MCN),which leads to rapid separation and transfer of photogenerated charge carriers.The polymerization of urea in the presence of KOH creates CN homojunction with amino and cyano groups.The subsequent molten salt treatment induces a new type of cyano-terminated CN that can be converted to MCN through photodoping,forming homojunction and ohmic contact coexisting CN(HOCN).The formed HOCN photocatalyst exhibits a high photocatalytic H_(2)evolution rate of 18.5 mmol·g^(-1)·h^(-1)under visible light irradiation,45-fold higher than that of bulk CN.This strategy provides a new idea for designing ohmic contact between semiconductor and metal,and realizing efficient photocatalysis by improving charge separation and transfer.

关键词： carbon nitride photocatalysis homojunction ohmic contact hydrogen evolution