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Insight into structure evolution of carbon nitrides and its energy conversion as luminescence
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作者 Hao Zhang Jingwei Zhang +4 位作者 Wenjie Chen Minjia Tao Xianguang Meng Yuanjian Zhang Guifu Zuo 《Carbon Energy》 SCIE EI CAS CSCD 2024年第2期37-60,共24页
A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C3N4)have been widely used in bioimaging,biosensing,and other fields in recent years due to their nontoxicity,low cost,and high lumines... A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C3N4)have been widely used in bioimaging,biosensing,and other fields in recent years due to their nontoxicity,low cost,and high luminescent quantum efficiency.What is more attractive is that the luminescent properties such as wavelength and intensity can be regulated by controlling the structure at the molecular level.Hence,it is time to summarize the related research on CN structural evolution and make a prospect on future developments.In this review,we first summarize the research history and multiple structural evolution of CN.Then,the progress of improving the luminescence performance of CN through structural evolution was discussed.Significantly,the relationship between CN structure evolution and energy conversion in the forms of photoluminescence,chemiluminescence,and electrochemiluminescence was reviewed.Finally,key challenges and opportunities such as nanoscale dispersion strategy,luminous efficiency improving methods,standardization evaluation,and macroscopic preparation of CN are highlighted. 展开更多
关键词 carbon nitride CHEMILUMINESCENCE ELECTROCHEMILUMINESCENCE energy conversion PHOTOLUMINESCENCE structural evolution
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Improved Plasmonic Hot‑Electron Capture in Au Nanoparticle/Polymeric Carbon Nitride by Pt Single Atoms for Broad‑Spectrum Photocatalytic H_(2)Evolution 被引量:2
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作者 Manyi Gao Fenyang Tian +3 位作者 Xin Zhang Zhaoyu Chen Weiwei Yang Yongsheng Yu 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第8期423-435,共13页
ABSTRACT Rationally designing broad-spectrum photocatalysts to harvest whole visible-light region photons and enhance solar energy conversion is a“holy grail”for researchers,but is still a challenging issue.Herein,b... ABSTRACT Rationally designing broad-spectrum photocatalysts to harvest whole visible-light region photons and enhance solar energy conversion is a“holy grail”for researchers,but is still a challenging issue.Herein,based on the common polymeric carbon nitride(PCN),a hybrid co-catalysts system comprising plasmonic Au nanoparticles(NPs)and atomically dispersed Pt single atoms(PtSAs)with different functions was constructed to address this challenge.For the dual co-catalysts decorated PCN(PtSAs–Au_(2.5)/PCN),the PCN is photoexcited to generate electrons under UV and short-wavelength visible light,and the synergetic Au NPs and PtSAs not only accelerate charge separation and transfer though Schottky junctions and metal-support bond but also act as the co-catalysts for H_(2) evolution.Furthermore,the Au NPs absorb long-wavelength visible light owing to its localized surface plasmon resonance,and the adjacent PtSAs trap the plasmonic hot-electrons for H_(2) evolution via direct electron transfer effect.Consequently,the PtSAs–Au_(2.5)/PCN exhibits excellent broad-spectrum photocatalytic H_(2) evolution activity with the H_(2) evolution rate of 8.8 mmol g^(−1) h^(−1) at 420 nm and 264μmol g^(−1) h^(−1) at 550 nm,much higher than that of Au_(2.5)/PCN and PtSAs–PCN,respectively.This work provides a new strategy to design broad-spectrum photocatalysts for energy conversion reaction. 展开更多
关键词 Polymeric carbon nitride Au nanoparticles Pt single atoms Photocatalytic H2 evolution Broad-spectrum photocatalysts
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Carbon Nitride Quantum Dots:A Novel Fluorescent Probe for Non-Enzymatic Hydrogen Peroxide and Mercury Detection 被引量:1
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作者 CHEN Lei LI Quan +2 位作者 WANG Xing WANG Wentai WANG Lisha 《Journal of Ocean University of China》 SCIE CAS CSCD 2023年第6期1572-1582,共11页
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... 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. 展开更多
关键词 carbon nitride quantum dots hydrogen peroxide Hg2+ fluorescence probe
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Composite polymer electrolyte reinforced by graphitic carbon nitride nanosheets for room-temperature all-solid-state lithium batteries
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作者 Qingyue Han Suqing Wang +2 位作者 Wenhan Kong Bing Ji Haihui Wang 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2023年第2期257-263,共7页
By virtue of the flexibility and safety, polyethylene oxide(PEO) based electrolytes are regarded as an appealing candidate for all-solid-state lithium batteries. However, their application is limited by the poor ionic... By virtue of the flexibility and safety, polyethylene oxide(PEO) based electrolytes are regarded as an appealing candidate for all-solid-state lithium batteries. However, their application is limited by the poor ionic conductivity at room temperature, narrow electrochemical stability window and uncontrolled growth of lithium dendrite. To alleviate these problems, we introduce the ultrathin graphitic carbon nitride nanosheets(GCN) as advanced nanofillers into PEO based electrolytes(GCN-CPE). Benefiting from the high surface area and abundant surface N-active sites of GCN, the GCN-CPE displays decreased crystallinity and enhanced ionic conductivity. Meanwhile, Fourier transform infrared and chronoamperometry studies indicate that GCN can facilitate Li+migration in the composite electrolyte. Additionally, the GCN-CPE displays an extended electrochemical window compared with PEO based electrolytes. As a result, Li symmetric battery assembled with GCN-CPE shows a stable Li plating/stripping cycling performance, and the all-solid-state Li/LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622) batteries using GCN-CPE exhibit satisfactory cyclability and rate capability in a voltage range of 3-4.2 V at 30 ℃. 展开更多
关键词 Electrolytes POLYMERS Graphitic carbon nitride nanosheets Composites Room temperature All-solid-state battery
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Smart Interfacing between Co-Fe Layered Double Hydroxide and Graphitic Carbon Nitride for High-efficiency Electrocatalytic Nitrogen Reduction
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作者 Xiaohui Wu Lu Tang +5 位作者 Yang Si Chunlan Ma Peng Zhang Jianyong Yu Yitao Liu Bin Ding 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第2期62-69,共8页
Bimetallic compounds such as hydrotalcite-type layered double hydroxides(LDHs)are promising electrocatalysts owing to their unique electronic structures.However,their abilities toward nitrogen adsorption and reduction... Bimetallic compounds such as hydrotalcite-type layered double hydroxides(LDHs)are promising electrocatalysts owing to their unique electronic structures.However,their abilities toward nitrogen adsorption and reduction are undermined since the surface-mantled,electronegative-OH groups hinder the charge transfer between transition metal atoms and nitrogen molecules.Herein,a smart interfacing strategy is proposed to construct a coupled heterointerface between LDH and 2D g-C_(3)N_(4),which is proven by density functional theory(DFT)investigations to be favorable for nitrogen adsorption and ammonia desorption compared with neat LDH surface.The interfaced LDH and g-C_(3)N_(4) is further hybridized with a self-standing TiO_(2) nanofibrous membrane(NM)to maximize the interfacial effect owing to its high porosity and large surface area.Profited from the synergistic superiorities of the three components,the LDH@C_(3)N_(4)@TiO_(2) NM delivers superior ammonia yield(2.07×10^(−9) mol s^(−1) cm^(−2))and Faradaic efficiency(25.3%),making it a high-efficiency,noble-metal-free catalyst system toward electrocatalytic nitrogen reduction. 展开更多
关键词 density functional theory electrocatalytic nitrogen reduction graphitic carbon nitride interface engineering layered double hydroxide
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Recent advances in graphitic carbon nitride-based photocatalysts for solar-driven hydrogen production
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作者 Zhihuan Miao Guanyu Wu +7 位作者 Qi Wang Jinman Yang Zeyu Wang Pengcheng Yan Peipei Sun Yucheng Lei Zhao Mo Hui Xu 《Materials Reports(Energy)》 EI 2023年第4期19-38,共20页
Due to the abundance and sustainability of solar energy,converting it into chemical energy to obtain clean energy presents an ideal solution for addressing environmental pollution and energy shortages stemming from th... Due to the abundance and sustainability of solar energy,converting it into chemical energy to obtain clean energy presents an ideal solution for addressing environmental pollution and energy shortages stemming from the extensive combustion of fossil fuels.In recent years,hydrogen energy has emerged on the stage of history as the most promising clean energy carrier of the 21st century.Among the current methods of producing hydrogen,photocatalytic hydrogen production technology,as a zero-carbon approach to producing high calorific value and pollution-free hydrogen energy,has attracted much attention since its discovery.As the core of photocatalysis technology,semiconductor photocatalysts are always the research hotspots.Among them,graphite-phase carbon nitride(g-C_(3)N_(4)),an organic semiconductor material composed of only C and N elements,possesses physicochemical properties incomparable to those of traditional inorganic semiconductor materials,including suitable energy band positions,easy structural regulation,inexpensive raw materials and abundant reserves,simple preparation,high thermal/mechanical/chemical stability,etc.Therefore,g-C_(3)N_(4) has attracted extensive attention in the field of photocatalytic hydrogen production in the last two decades.This review comprehensively outlines the research trajectory of g-C_(3)N_(4) photocatalytic hydrogen production,encompassing development,preparation methods,advantages,and disadvantages.A concise introduction to g-C_(3)N_(4) is provided,as well as an analysis of the underlying mechanism of the photocatalytic system.Additionally,it delves into the latest techniques to enhance performance,including nanostructure design,elemental doping,and heterojunction construction.The applications of g-C_(3)N_(4) based photocatalysts in hydrogen production are surveyed,underscoring the significance of catalyst active sites and g-C_(3)N_(4) synthesis pathways.At length,concluded are insights into the challenges and opportunities presented by g-C_(3)N_(4) based photocatalysts for achieving heightened hydrogen production. 展开更多
关键词 carbon nitride PHOTOCATALYSIS Hydrogen evolution NANOSTRUCTURES DOPING HETEROJUNCTIONS
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Intrinsic Mechanisms of Morphological Engineering and Carbon Doping for Improved Photocatalysis of 2D/2D Carbon Nitride Van Der Waals Heterojunction
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作者 Jinqiang Zhang Xiaoli Zhao +10 位作者 Lin Chen Shuli Li Haijun Chen Yuezhao Zhu Shuaijun Wang Yang Liu Huayang Zhang Xiaoguang Duan Mingbo Wu Shaobin Wang Hongqi Sun 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第3期96-106,共11页
Van der Waals(VDW)heterojunctions in a 2D/2D contact provide the highest area for the separation and transfer of charge carriers.In this work,a top-down strategy with a gas erosion process was employed to fabricate a ... Van der Waals(VDW)heterojunctions in a 2D/2D contact provide the highest area for the separation and transfer of charge carriers.In this work,a top-down strategy with a gas erosion process was employed to fabricate a 2D/2D carbon nitride VDW heterojunction in carbon nitride(g-C_(3)N_(4))with carbon-rich carbon nitride.The created 2D semiconducting channel in the VDW structure exhibits enhanced electric field exposure and radiation absorption,which facilitates the separation of the charge carriers and their mobility.Consequently,compared with bulk g-C_(3)N_(4)and its nanosheets,the photocatalytic performance of the fabricated carbon nitride VDW heterojunction in the water splitting reaction to hydrogen is improved by 8.6 and 3.3 times,respectively,while maintaining satisfactory photo-stability.Mechanistically,the finite element method(FEM)was employed to evaluate and clarify the contributions of the formation of VDW heterojunction to enhanced photocatalysis,in agreement quantitatively with experimental ones.This study provides a new and effective strategy for the modification and more insights to performance improvement on polymeric semiconductors in photocatalysis and energy conversion. 展开更多
关键词 carbon nitride Van der Waals heterojunctions enhanced electric field exposure improved radiation absorption photocatalytic water splitting promoted dynamics of charge carriers
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Construction of Fluorescence Sensing Platform on the Basis of Carbon Nitride Nanosheet for the Detection of Interferon-γ
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作者 Xiaoqing Wen Zichun Song +3 位作者 Jiuying Cui Yan Li Qianli Tang Xianjiu Liao 《Journal of Biosciences and Medicines》 CAS 2023年第1期162-174,共13页
Purpose: Interferon-γ (INF-γ) is a cytokine that participates in the immune reaction of the body. Its level of secretion can reflect the immune response condition after the body is infected by pathogens, which is a ... Purpose: Interferon-γ (INF-γ) is a cytokine that participates in the immune reaction of the body. Its level of secretion can reflect the immune response condition after the body is infected by pathogens, which is a significant indication of clinically-related diseases. Therefore, it is of great significance in application to develop a fluorescence biosensor to inspect INF-γ with rapidness, high sensitivity and high practicability. Method: The fluorescence sensor is made on the basis of the two-dimensional nano-material namely Carbon Nitride Nanosheet (CNNS) and the Aptamer probe to identify INF-γ (Apt&reg;INF-γ). CNNS can quickly quench the Cy5 fluorescent dye modified on the Apt&reg;INF-γ probe due to the Photoinduced Electron Transfer (PET), but when the INF-γ exists, Apt&reg;INF-γ specifically identifies and combines it. The complex of Apt&reg;INF-γ and INF-γ is away from CNNS, which can effectively block the fluorescent signal of Apt?INF-γ being quenched by CNNS. Result: The sensitive detection of IFN-γ protein can be achieved through the application of CNNS/Apt&reg;INF-γ fluorescence sensing platform. In this method, the intensity of the fluorescent signal is positively correlated with the concentration of IFN-γ, of which the liner response range is 0.5 - 100 ng/mL and the limit of detection is 0.303 ng/mL. In addition, this fluorescence sensing platform has the advantages of high specificity, simple operation and low costs. It can inspect the content of IFN-γ in clinical serum samples without interference. The actual recovery rate of serum samples is 97.11% - 106.96%. Conclusion: Therefore, the CNNS/Apt&reg;INF-γ sensing platform is expected to be implemented in the actual clinical detection, also conducive to developing a universal fluorescence biosensor to inspect other target materials. 展开更多
关键词 carbon nitride Nanosheet APTAMER INTERFERON-Γ Fluorescence Sensing Analysis
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Recent Advances of Graphitic Carbon Nitride-Based Structures and Applications in Catalyst, Sensing, Imaging, and LEDs 被引量:9
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作者 Aiwu Wang Chundong Wang +2 位作者 Li Fu Winnie Wong-Ng Yucheng Lan 《Nano-Micro Letters》 SCIE EI CAS 2017年第4期108-128,共21页
The graphitic carbon nitride(g-C_3N_4) which is a two-dimensional conjugated polymer has drawn broad interdisciplinary attention as a low-cost, metal-free, and visible-light-responsive photocatalyst in the area of env... The graphitic carbon nitride(g-C_3N_4) which is a two-dimensional conjugated polymer has drawn broad interdisciplinary attention as a low-cost, metal-free, and visible-light-responsive photocatalyst in the area of environmental remediation. The g-C_3N_4-based materials have excellent electronic band structures, electron-rich properties, basic surface functionalities, high physicochemical stabilities and are ‘‘earth-abundant.'' This review summarizes the latest progress related to the design and construction of g-C_3N_4-based materials and their applications including catalysis, sensing,imaging, and white-light-emitting diodes. An outlook on possible further developments in g-C_3N_4-based research for emerging properties and applications is also included. 展开更多
关键词 Graphitic carbon nitride(g-C3N4) CATALYSIS SENSING IMAGING LED
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Energy-level dependent H_2_O_2 production on metal-free,carbon-content tunable carbon nitride photocatalysts 被引量:4
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作者 Ruirui Wang Xin Zhang +5 位作者 Fan Li Ding Cao Min Pu Dandan Han Junjiao Yang Xu Xiang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2018年第2期343-350,共8页
Light-driven production of H2O2 from water and molecular oxygen could be a promising way for obtaining both solar fuels and fundamental chemicals. During that process, the H2O2 yield is strongly dependent on the react... Light-driven production of H2O2 from water and molecular oxygen could be a promising way for obtaining both solar fuels and fundamental chemicals. During that process, the H2O2 yield is strongly dependent on the reaction pathway associated with two-electron reduction of dioxygen by the photo-generated electrons. Herein, we synthesized a series of metal-free, carbon-content tunable carbon nitride photocatalysts(named C3N4-Carbon) by a facile hydrothermal reaction and subsequent thermal treatment at appropriate temperatures. The energy levels of the C3N4-Carbon catalysts vary with the carbon doping level, which is conveniently tuned by changing the initial glucose concentration during the hydrothermal reaction. The surface carbon species evolve with the carbon content and the nitrogen atoms in the structure of carbon nitride are partially substituted by foreign carbon atoms based on XPS measurements. The optimal catalyst leads to the highest H2O2 yield of 1271 μmol L-1 in an acidic aqueous solution(pH 3) after a reaction period of 4 h, twice higher than the pristine C3N4. In addition, the largest formation rate constant and the smallest decomposition rate constant of H2O2 are obtained on the optimal one according to the kinetics analyses. The decomposition tests of H2O2 indicate that the formation rate could be a dominant factor impacting the H2O2 yield. The conduction band position of the optimal catalyst is positively shifted to 0.06 V versus RHE, which is more favorable to the reduction of dioxygen to H2O2(O2/H2O2 at 0.69 V versus RHE). The positive shift of valence band also improves hole collection and leads to enhanced formation of H2O2. 展开更多
关键词 Hydrogen peroxide PHOTOCATALYSIS carbon nitride Oxygen reduction Kinetics
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Monolayer Graphitic Carbon Nitride as Metal-Free Catalyst with Enhanced Performance in Photo- and Electro-Catalysis 被引量:5
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作者 Huiyan Piao Goeun Choi +4 位作者 Xiaoyan Jin Seong‑Ju Hwang Young Jae Song Sung‑Pyo Cho Jin‑Ho Choy 《Nano-Micro Letters》 SCIE EI CAS CSCD 2022年第3期308-321,共14页
The exfoliation of bulk graphitic carbon nitride(g-C_(3)N_(4))into monolayer has been intensively studied to induce maximum sur-face area for fundamental studies,but ended in failure to realize chemi-cally and physica... The exfoliation of bulk graphitic carbon nitride(g-C_(3)N_(4))into monolayer has been intensively studied to induce maximum sur-face area for fundamental studies,but ended in failure to realize chemi-cally and physically well-defined monolayer of g-C_(3)N_(4)mostly due to the difficulty in reducing the layer thickness down to an atomic level.It has,therefore,remained as a challenging issue in two-dimensional(2D)chemistry and physics communities.In this study,an“atomic monolayer of g-C_(3)N_(4)with perfect two-dimensional limit”was successfully prepared by the chemically well-defined two-step routes.The atomically resolved monolayer of g-C_(3)N_(4)was also confirmed by spectroscopic and micro-scopic analyses.In addition,the experimental Cs-HRTEM image was collected,for the first time,which was in excellent agreement with the theoretically simulated;the evidence of monolayer of g-C_(3)N_(4)in the perfect 2D limit becomes now clear from the HRTEM image of orderly hexagonal symmetry with a cavity formed by encirclement of three adjacent heptazine units.Compared to bulk g-C_(3)N_(4),the present g-C_(3)N_(4)monolayer showed significantly higher photocatalytic gen-eration of H2O2 and H2,and electrocatalytic oxygen reduction reaction.In addition,its photocatalytic efficiency for H2O2 production was found to be the best for any known g-C_(3)N_(4)nanomaterials,underscoring the remarkable advantage of monolayer formation in optimizing the catalyst performance of g-C_(3)N_(4). 展开更多
关键词 Graphitic carbon nitride MONOLAYER Atomic image Electro-and photo-catalysis
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Electron-Deficient Zn-N_(6) Configuration Enabling Polymeric Carbon Nitride for Visible-Light Photocatalytic Overall Water Splitting 被引量:4
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作者 Daming Zhao Yiqing Wang +6 位作者 Chung-Li Dong Fanqi Meng Yu-Cheng Huang Qinghua Zhang Lin Gu Lan Liu Shaohua Shen 《Nano-Micro Letters》 SCIE EI CAS CSCD 2022年第12期602-616,共15页
Despite of suitable band structures for harvesting solar light and driving water redox reactions,polymeric carbon nitride(PCN)has suffered from poor charge transfer ability and sluggish surface reaction kinetics,which... Despite of suitable band structures for harvesting solar light and driving water redox reactions,polymeric carbon nitride(PCN)has suffered from poor charge transfer ability and sluggish surface reaction kinetics,which limit its photocatalytic activity for water splitting.Herein,atomically dispersed Zn-coordinated three-dimensional(3D)sponge-like PCN(Zn-PCN)is synthesized through a novel intermediate coordination strategy.Advanced characterizations and theoretical calculations well evidence that Zn single atoms are coordinated and stabilized on PCN in the form of Zn-N_(6) configura-tion featured with an electron-deficient state.Such an electronic configuration has been demonstrated contributive to promoted electron excitation,accelerated charge separation and transfer as well as reduced water redox barriers.Further benefited from the abundant surface active sites derived from the 3D porous structure,Zn-PCN realizes visible-light photocatalysis for overall water splitting with H_(2) and O_(2) simultaneously evolved at a stoichiometric ratio of 2:1.This work brings new insights into the design of novel single-atom photocatalysts by deepening the understanding of electronic configurations and reactive sites favorable to excellent photocatalysis for water splitting and related solar energy conversion reactions. 展开更多
关键词 Zn single atoms Polymeric carbon nitride Overall water splitting PHOTOCATALYSIS
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Constructing 3D interweaved MXene/graphitic carbon nitride nanosheets/graphene nanoarchitectures for promoted electrocatalytic hydrogen evolution 被引量:3
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作者 Haiyan He Yuxian Chen +3 位作者 Cuizhen Yang Lu Yang Quanguo Jiang Huajie Huang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第4期483-491,共9页
The technique of electrocatalytic hydrogen evolution reaction (HER) represents a development trend of clean energy generation and conversion,while the electrode catalysts are bound to be the core unit in the electroch... The technique of electrocatalytic hydrogen evolution reaction (HER) represents a development trend of clean energy generation and conversion,while the electrode catalysts are bound to be the core unit in the electrochemical HER system.Herein,we demonstrate a bottom-up approach to the construction of three-dimensional (3D) interconnected ternary nanoarchitecture originated from Ti_(3)C_(2)T_(x)MXene,graphitic carbon nitride nanosheets and graphene (MX/CN/RGO) through a convenient co-assembly process.By virtue of the 3D porous frameworks with ultrathin walls,large specific surface areas,optimized electronic structures,high electric conductivity,the resulting MX/CN/RGO nanoarchitecture expresses an exceptional HER performance with a low onset potential of only 38 m V,a small Tafel slop of 76 m V dec^(-1) as well as long lifespan,all of which are more competitive than those of the bare Ti_(3)C_(2)T_(x),g-C_(3)N_(4),graphene as well as binary MX/RGO and CN/RGO electrocatalysts.Theoretical simulations further verify that the ternary MX/CN/RGO nanoarchitecture with ameliorative band structure is able to facilitate the electron transport and meanwhile offer multistage catalytically active sites,thereby guaranteeing rapid HER kinetics during the electrocatalytic process. 展开更多
关键词 MXene carbon nitride GRAPHENE ELECTROCATALYSTS Hydrogen evolution
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Band Engineering and Morphology Control of Oxygen‑Incorporated Graphitic Carbon Nitride Porous Nanosheets for Highly Efficient Photocatalytic Hydrogen Evolution 被引量:3
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作者 Yunyan Wu Pan Xiong +7 位作者 Jianchun Wu Zengliang Huang Jingwen Sun Qinqin Liu Xiaonong Cheng Juan Yang Junwu Zhu Yazhou Zhou 《Nano-Micro Letters》 SCIE EI CAS CSCD 2021年第3期95-106,共12页
Graphitic carbon nitride(g-C3N4)-based photocatalysts have shown great potential in the splitting of water.However,the intrinsic drawbacks of g-C3N4,such as low surface area,poor diffusion,and charge separation effici... Graphitic carbon nitride(g-C3N4)-based photocatalysts have shown great potential in the splitting of water.However,the intrinsic drawbacks of g-C3N4,such as low surface area,poor diffusion,and charge separation efficiency,remain as the bottleneck to achieve highly efficient hydrogen evolution.Here,a hollow oxygen-incorporated g-C3N4 nanosheet(OCN)with an improved surface area of 148.5 m2 g^−1 is fabricated by the multiple thermal treatments under the N2/O2 atmosphere,wherein the C–O bonds are formed through two ways of physical adsorption and doping.The physical characterization and theoretical calculation indicate that the O-adsorption can promote the generation of defects,leading to the formation of hollow morphology,while the O-doping results in reduced band gap of g-C3N4.The optimized OCN shows an excellent photocatalytic hydrogen evolution activity of 3519.6μmol g^−1 h^−1 for~20 h,which is over four times higher than that of g-C3N4(850.1μmol g^−1 h^−1)and outperforms most of the reported g-C3N4 catalysts. 展开更多
关键词 Graphitic carbon nitride nanosheet Hollow morphology Oxygen incorporating Multiple thermal treatment Photocatalytic hydrogen evolution
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Heteropolyacids-Immobilized Graphitic Carbon Nitride:Highly Efficient Photo-Oxidation of Benzyl Alcohol in the Aqueous Phase 被引量:3
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作者 Lifu Wu Sai An Yu-Fei Song 《Engineering》 SCIE EI 2021年第1期94-102,共9页
Benzaldehyde is a highly desirable chemical due to its extensive application in medicine,chemical synthesis and food sector among others.However,its production generally involves hazardous solvents such as trifluoroto... Benzaldehyde is a highly desirable chemical due to its extensive application in medicine,chemical synthesis and food sector among others.However,its production generally involves hazardous solvents such as trifluorotoluene or acetonitrile,and its conversion,especially selectivity in the aqueous phase,is still not up to expectations.Hence,developing an environmentally benign,synthetic process for benzaldehyde production is of paramount importance.Herein,we report the preparation of a photocatalyst(PW_(12)-P-UCNS,where PW_(12)is H3PW_(12)O_(40)xH_(2)O and P-UCNS is phosphoric acid-modified unstack graphitic carbon nitride)by incorporating phosphotungstic acid on phosphoric acid-functionalised graphitic carbon nitride(g-C_(3)N_(4))nanosheets.The performance of PW_(12)-P-UCNS was tested using the benzyl alcohol photo-oxidation reaction to produce benzaldehyde in H_(2)O,at room temperature(20℃).The asprepared PW12-P-UCNS photocatalyst showed excellent photocatalytic performance with 58.3%conversion and 99.5%selectivity within 2 h.Moreover,the catalyst could be reused for at least five times without significant activity loss.Most importantly,a proposed Z-scheme mechanism of the PW_(12)-P-UCNScatalysed model reaction was revealed.We carefully investigated its transient photocurrent and electrochemical impedance,and identified superoxide radicals and photogenerated holes as the main active species through electron spin-resonance spectroscopy and scavenger experiments.Results show that the designed PW_(12)-P-UCNS photocatalyst is a highly promising candidate for benzaldehyde production through the photo-oxidation reaction in aqueous phase,under mild conditions. 展开更多
关键词 Photocatalysis HETEROPOLYACIDS Graphitic carbon nitride BENZALDEHYDE
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Nitrogen-doped Carbon Nanospheres-Modified Graphitic Carbon Nitride with Outstanding Photocatalytic Activity 被引量:3
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作者 Qiaoran Liu Hao Tian +6 位作者 Zhenghua Dai Hongqi Sun Jian Liu Zhimin Ao Shaobin Wang Chen Han Shaomin Liu 《Nano-Micro Letters》 SCIE EI CAS CSCD 2020年第2期154-168,共15页
Metals and metal oxides are widely used as photo/electro-catalysts for environmental remediation.However,there are many issues related to these metal-based catalysts for practical applications,such as high cost and de... Metals and metal oxides are widely used as photo/electro-catalysts for environmental remediation.However,there are many issues related to these metal-based catalysts for practical applications,such as high cost and detrimental environmental impact due to metal leaching.Carbon-based catalysts have the potential to overcome these limitations.In this study,monodisperse nitrogen-doped carbon nanospheres(NCs)were synthesized and loaded onto graphitic carbon nitride(g-C3N4,GCN)via a facile hydrothermal method for photocatalytic removal of sulfachloropyridazine(SCP).The prepared metal-free GCN-NC exhibited remarkably enhanced efficiency in SCP degradation.The nitrogen content in NC critically influences the physicochemical properties and performances of the resultant hybrids.The optimum nitrogen doping concentration was identified at 6.0 wt%.The SCP removal rates can be improved by a factor of 4.7 and 3.2,under UV and visible lights,by the GCN-NC composite due to the enhanced charge mobility and visible light harvesting.The mechanism of the improved photocatalytic performance and band structure alternation were further investigated by density functional theory(DFT)calculations.The DFT results confirm the high capability of the GCN-NC hybrids to activate the electron–hole pairs by reducing the band gap energy and efficiently separating electron/hole pairs.Superoxide and hydroxyl radicals are subsequently produced,leading to the efficient SCP removal. 展开更多
关键词 N-DOPING carbon sphere Graphitic carbon nitride PHOTOCATALYSIS DEGRADATION
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Graphitic carbon nitride (g-C3N4)-based nanosized heteroarrays: Promising materials for photoelectrochemical water splitting 被引量:10
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作者 Liqun Wang Wenping Si +6 位作者 Yueyu Tong Feng Hou Daniele Pergolesi Jungang Hou Thomas Lippert Shi Xue Dou Ji Liang 《Carbon Energy》 CAS 2020年第2期223-250,共28页
Photoelectrochemical(PEC)water splitting is recognized as a sustainable strategy for hydrogen generation due to its abundant hydrogen source,utilization of inexhaustible solar energy,high-purity product,and environmen... Photoelectrochemical(PEC)water splitting is recognized as a sustainable strategy for hydrogen generation due to its abundant hydrogen source,utilization of inexhaustible solar energy,high-purity product,and environment-friendly process.To actualize a practical PEC water splitting,it is paramount to develop efficient,stable,safe,and low-cost photoelectrode materials.Recently,graphitic carbon nitride(g-C3N4)has aroused a great interest in the new generation photoelectrode materials because of its unique features,such as suitable band structure for water splitting,a certain range of visible light absorption,nontoxicity,and good stability.Some inherent defects of g-C3N4,however,seriously impair further improvement on PEC performance,including low electronic conductivity,high recombination rate of photogenerated charges,and limited visible light absorption at long wavelength range.Construction of g-C3N4-based nanosized heteroarrays as photoelectrodes has been regarded as a promising strategy to circumvent these inherent limitations and achieve the high-performance PEC water splitting due to the accelerated exciton separation and the reduced combination of photogenerated electrons/holes.Herein,we summarize in detail the latest progress of g-C3N4-based nanosized heteroarrays in PEC water-splitting photoelectrodes.Firstly,the unique advantages of this type of photoelectrodes,including the highly ordered nanoarray architectures and the heterojunctions,are highlighted.Then,different g-C3N4-based nanosized heteroarrays are comprehensively discussed,in terms of their fabrication methods,PEC capacities,and mechanisms,etc.To conclude,the key challenges and possible solutions for future development on g-C3N4-based nanosized heteroarray photoelectrodes are discussed. 展开更多
关键词 graphitic carbon nitride HETEROJUNCTIONS NANOARRAYS photoelectrochemical water splitting
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Multidimensional(0D-3D)functional nanocarbon:Promising material to strengthen the photocatalytic activity of graphitic carbon nitride 被引量:3
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作者 Bin He Mi Feng +1 位作者 Xinyan Chen Jian Sun 《Green Energy & Environment》 SCIE CSCD 2021年第6期823-845,共23页
As a prospective visible-light-responsive photochemical material,graphitic carbon nitride(g-C_(3)N_(4))has become a burgeoning research hot topics and aroused a wide interest as a metal-free semiconductor in the area ... As a prospective visible-light-responsive photochemical material,graphitic carbon nitride(g-C_(3)N_(4))has become a burgeoning research hot topics and aroused a wide interest as a metal-free semiconductor in the area of energy utilization and conversion,environmental protection due to its unique properties,such as facile synthesis,high physicochemical stability,excellent electronic band structure,and sustainability.However,the shortcomings of high recombination rate of charge carriers,relatively low electrical conductivity and visible light absorption impede its practical application.Various strategies,such as surface photosensitization,heteroatom deposition,semiconductor hybridization,etc.,have been applied to overcome the barriers.Among all the strategies,functional nanocarbon materials with various dimensions(0D~3D)attract much attention as modifiers of g-C_(3)N_(4)due to their unique electronic properties,optical properties,and easy functionalization.More importantly,the properties of these functional nanocarbon materials can be tuned by various dimensions and thus there will be a way to overcome the defects of g-C_(3)N_(4)by choosing different dimensional carbon materials.Distinguishing from some present reviews,this review starts with the fundamental physicochemical characteristics of g-C_(3)N_(4)materials,followed by analyzing the advantages of functional nanocarbon materials modifying gC_(3)N_(4).Then,we present a systematic introduction to various dimensional carbon materials.The design philosophy of carbon/g-C_(3)N_(4)composites and the advanced studies are exemplified in detail.Finally,a nichetargeting summary and outlook on the major challenges,opportunities for future research in high-powered carbon/g-C_(3)N_(4)composites was proposed. 展开更多
关键词 Graphitic carbon nitride(g-C_(3)N_(4)) carbon materials Multidimension PHOTOCATALYSIS Visible light
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Pomelo biochar as an electron acceptor to modify graphitic carbon nitride for boosting visible-light-driven photocatalytic degradation of tetracycline 被引量:2
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作者 Feng Guo Chunli Shi +3 位作者 Wei Sun Yanan Liu Xue Lin Weilong Shi 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2022年第8期1-11,共11页
In this study,biochar(BC)derived from pomelo was prepared via a high-temperature calcination method to modify the graphitic carbon nitride(g-C_(3)N_(4))to synthesize the BC/g-C_(3)N_(4)composite for the degradation of... In this study,biochar(BC)derived from pomelo was prepared via a high-temperature calcination method to modify the graphitic carbon nitride(g-C_(3)N_(4))to synthesize the BC/g-C_(3)N_(4)composite for the degradation of the tetracycline(TC)antibiotic under visible light irradiation.The experimental results exhibit that the optimal feeding weight ratio of biochar/urea is 0.03:1 in BC/g-C_(3)N_(4)composite could show the best photocatalytic activity with the degradation rate of tetracycline is 83%in 100 min irradiation.The improvement of photocatalytic activity is mainly attributed to the following two points:(i)the strong bonding with π-π stacking between BC and g-C_(3)N_(4)make the photogenerated electrons of light-excited g-C_(3)N_(4)transfer to BC,quickly and improve the separation efficiency of carriers;(ii)the introduction of BC reduces the distance for photogenerated electrons to migrate to the surface and increases the specific surface area for providing more active sites.This study provides a sustainable,economical and promising method for the synthesis of photocatalytic materials their application to wastewater treatment. 展开更多
关键词 POMELO BIOCHAR Graphitic carbon nitride Photocatalytic degradation Electron acceptor
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Hierarchical Self-assembly of Well-Defined Louver-Like P-Doped Carbon Nitride Nanowire Arrays with Highly Effcient Hydrogen Evolution 被引量:2
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作者 Bo Li Yuan Si +6 位作者 Qian Fang Ying Shi Wei‑Qing Huang Wangyu Hu Anlian Pan Xiaoxing Fan Gui‑Fang Huang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2020年第4期76-91,共16页
Self-assembled nanostructure arrays integrating the advantages of the intrinsic characters of nanostructure as well as the array stability are appealing in advanced materials.However,the precise bottom-up synthesis of... Self-assembled nanostructure arrays integrating the advantages of the intrinsic characters of nanostructure as well as the array stability are appealing in advanced materials.However,the precise bottom-up synthesis of nanostructure arrays without templates or substrates is quite challenging because of the general occurrence of homogeneous nucleation and the difficult manipulation of noncovalent interactions.Herein,we first report the precisely manipulated synthesis of well-defined louver-like P-doped carbon nitride nanowire arrays(L-PCN)via a supramolecular self-assembly method by regulating the noncovalent interactions through hydrogen bond.With this strategy,CN nanowires align in the outer frame with the separation and spatial location achieving ultrastability and outstanding photoelectricity properties.Significantly,this self-assembly L-PCN exhibits a superior visible light-driven hydrogen evolution activity of 1872.9μmol h^−1 g^−1,rendering a^25.6-fold enhancement compared to bulk CN,and high photostability.Moreover,an apparent quantum efficiency of 6.93%is achieved for hydrogen evolution at 420±15 nm.The experimental results and first-principles calculations demonstrate that the remarkable enhancement of photocatalytic activity of L-PCN can be attributed to the synergetic effect of structural topology and dopant.These findings suggest that we are able to design particular hierarchical nanostructures with desirable performance using hydrogen-bond engineering. 展开更多
关键词 SELF-ASSEMBLY carbon nitride P-doped Nanowire arrays Hydrogen evolution
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