A novel composite photocatalyst for photocatalytic decomposition of water for hydrogen evolution was successfully synthesized by in-situ growth of nitrogen and sulfur co-doped coal-based carbon quantum dots(NSCQDs)nan...A novel composite photocatalyst for photocatalytic decomposition of water for hydrogen evolution was successfully synthesized by in-situ growth of nitrogen and sulfur co-doped coal-based carbon quantum dots(NSCQDs)nanoparticles on the surface of sheet cobalt-based metal-organic framework(Co-MOF)and graphitic carbon nitride(g-C_(3)N_(4),CN).The structure and properties of the obtained catalysts were systematically analyzed.NSCQDs effectively broaden the absorption of Co-MOF and CN in the visible region.The new composite photocatalyst has high hydrogen production activity and the hydrogen production rate reaches 6254μmol/(g·h)at pH=9.At the same time,NSCQDs synergy Co-MOF/CN composites have good stability.After four cycles of hydrogen production,the performance remains relatively stable.The tran sient photocurrent response and Nyquist plot experimental results further demonstrate the improvement of carrier separation efficiency in composite catalysts.The semiconductor type(n-type semico nductor)of the single-phase catalyst was determined by the Mott-Schottky test,and the band structure was analyzed.The conductive and valence bands of CN are-0.99 and 1.72 eV,respectively,and the conduction and valence bands of Co-MOF are-1.85 and 1.33 eV,respectively.Th e mechanism of the photocatalytic reaction can be inferred,that is,Z-type heterojunction is formed between CN an d Co-MOF,and NSCQDs was used as cocatalyst.展开更多
As a novel zero-dimensional(0D)material,metal carbides and/or carbonitrides(MXenes)quantum dots(MQDs)show unique photoluminescence properties and excellent biocompatibility.However,due to the limited synthesis methods...As a novel zero-dimensional(0D)material,metal carbides and/or carbonitrides(MXenes)quantum dots(MQDs)show unique photoluminescence properties and excellent biocompatibility.However,due to the limited synthesis methods and research to date,many new features have yet to be uncovered.Here,to explore their new properties and expand biological applications,chlorine and nitrogen co-doped Ti_(3)C_(2)MXene quantum dots(Cl,N-Ti_(3)C_(2)MQDs)were designed and synthesized,and their hydroxyl radical scavenging properties were investigated for the first time,revealing outstanding performance.Cl,N-Ti_(3)C_(2)MQDs was directly stripped from bulk Ti_(3)Al C_(2)by electrochemical etching,while N and Cl are successfully introduced to carbon skeleton and Ti boundaries in the etching process by electrochemical reactions between selected electrolytes and Ti_(3)C_(2)skeleton,respectively.The obtained Cl,N-Ti_(3)C_(2)MQDs exhibit large surface-to-volume ratio due to small particle size(ca.3.45 nm)and excellent higher scavenging activity(93.3%)and lower usage(12.5μg/m L)towards hydroxyl radicals than the previous reported graphene-based nanoparticles.The underlying mechanism of scavenging activity was also studied based on the reduction experiment with potassium permanganate(KMnO_(4)).The reducing ability of the intrinsic Ti_(3)C_(2)structure and electron donation of double dopants are the main contributors to the outstanding scavenging activity.展开更多
Flexible and all-solid-state zinc-air batteries(ZABs)are highly useful and also in demand due to their theoretical high energy densities and special applications.The limitation in their performance arises due to their...Flexible and all-solid-state zinc-air batteries(ZABs)are highly useful and also in demand due to their theoretical high energy densities and special applications.The limitation in their performance arises due to their catalyst-coated cathode electrodes in terms of catalytic activity and stability as well as cost.In this paper,a novel and environmentally friendly activation strategy is developed to activate the carbon cloth(CC)for the electrodes.The activated CC serves as a catalyst-free air cathode with high conductivity,excellent mechanical strength,and flexibility,in addition to low cost.The strategy is performed by simply electro-oxidizing and electroreducing CC under ultrahigh direct current(DC)voltage in a diluted NH4Cl aqueous electrolyte.It is found that the electro-oxidation not only results in the formation of a graphene-like exfoliated carbon layer on the surface of CC but also induces the incorporation of oxygen-containing groups and doping of nitrogen and chloride atoms.After the electroreduction,theπ-conjugated carbon network of CC is partially restored,leading to the recovery of electroconductivity.Such an electroactivated CC shows excellent oxygen reduction reaction activity.The aqueous flexibility and all-solid-state ZABs are assembled using such an electroactivated CC cathode without any catalyst loading.Both ZABs can achieve good durability and deliver high peak power density and an energy density as high as 690 Wh kg^(−1),demonstrating the excellent potential of this electroactivated CC in practical devices.展开更多
基金Project supported by the Ningxia Natural Science Foundation of China(2023AAC03285)National Natural Science Foundation of China(21666001)+1 种基金Innovative Team for Transforming Waste Cooking Oil into Clean Energy and High Value-added Chemicals,ChinaNingxia Low-grade Resource High Value Utilization and Environmental Chemical Integration Technology Innovation Team Project,China。
文摘A novel composite photocatalyst for photocatalytic decomposition of water for hydrogen evolution was successfully synthesized by in-situ growth of nitrogen and sulfur co-doped coal-based carbon quantum dots(NSCQDs)nanoparticles on the surface of sheet cobalt-based metal-organic framework(Co-MOF)and graphitic carbon nitride(g-C_(3)N_(4),CN).The structure and properties of the obtained catalysts were systematically analyzed.NSCQDs effectively broaden the absorption of Co-MOF and CN in the visible region.The new composite photocatalyst has high hydrogen production activity and the hydrogen production rate reaches 6254μmol/(g·h)at pH=9.At the same time,NSCQDs synergy Co-MOF/CN composites have good stability.After four cycles of hydrogen production,the performance remains relatively stable.The tran sient photocurrent response and Nyquist plot experimental results further demonstrate the improvement of carrier separation efficiency in composite catalysts.The semiconductor type(n-type semico nductor)of the single-phase catalyst was determined by the Mott-Schottky test,and the band structure was analyzed.The conductive and valence bands of CN are-0.99 and 1.72 eV,respectively,and the conduction and valence bands of Co-MOF are-1.85 and 1.33 eV,respectively.Th e mechanism of the photocatalytic reaction can be inferred,that is,Z-type heterojunction is formed between CN an d Co-MOF,and NSCQDs was used as cocatalyst.
基金National Natural Science Foundation of China(Grant No.21674011,21404008)Beijing Municipal Natural Science Foundation(Grant No.2172040)+1 种基金Beijing Organization department outstanding talented person project(2013D009006000001)the Fundamental Research Funds for the Central Universities(FRF-GF-17-B11)。
文摘As a novel zero-dimensional(0D)material,metal carbides and/or carbonitrides(MXenes)quantum dots(MQDs)show unique photoluminescence properties and excellent biocompatibility.However,due to the limited synthesis methods and research to date,many new features have yet to be uncovered.Here,to explore their new properties and expand biological applications,chlorine and nitrogen co-doped Ti_(3)C_(2)MXene quantum dots(Cl,N-Ti_(3)C_(2)MQDs)were designed and synthesized,and their hydroxyl radical scavenging properties were investigated for the first time,revealing outstanding performance.Cl,N-Ti_(3)C_(2)MQDs was directly stripped from bulk Ti_(3)Al C_(2)by electrochemical etching,while N and Cl are successfully introduced to carbon skeleton and Ti boundaries in the etching process by electrochemical reactions between selected electrolytes and Ti_(3)C_(2)skeleton,respectively.The obtained Cl,N-Ti_(3)C_(2)MQDs exhibit large surface-to-volume ratio due to small particle size(ca.3.45 nm)and excellent higher scavenging activity(93.3%)and lower usage(12.5μg/m L)towards hydroxyl radicals than the previous reported graphene-based nanoparticles.The underlying mechanism of scavenging activity was also studied based on the reduction experiment with potassium permanganate(KMnO_(4)).The reducing ability of the intrinsic Ti_(3)C_(2)structure and electron donation of double dopants are the main contributors to the outstanding scavenging activity.
基金National Nature Science Foundation of China,Grant/Award Number:21908124。
文摘Flexible and all-solid-state zinc-air batteries(ZABs)are highly useful and also in demand due to their theoretical high energy densities and special applications.The limitation in their performance arises due to their catalyst-coated cathode electrodes in terms of catalytic activity and stability as well as cost.In this paper,a novel and environmentally friendly activation strategy is developed to activate the carbon cloth(CC)for the electrodes.The activated CC serves as a catalyst-free air cathode with high conductivity,excellent mechanical strength,and flexibility,in addition to low cost.The strategy is performed by simply electro-oxidizing and electroreducing CC under ultrahigh direct current(DC)voltage in a diluted NH4Cl aqueous electrolyte.It is found that the electro-oxidation not only results in the formation of a graphene-like exfoliated carbon layer on the surface of CC but also induces the incorporation of oxygen-containing groups and doping of nitrogen and chloride atoms.After the electroreduction,theπ-conjugated carbon network of CC is partially restored,leading to the recovery of electroconductivity.Such an electroactivated CC shows excellent oxygen reduction reaction activity.The aqueous flexibility and all-solid-state ZABs are assembled using such an electroactivated CC cathode without any catalyst loading.Both ZABs can achieve good durability and deliver high peak power density and an energy density as high as 690 Wh kg^(−1),demonstrating the excellent potential of this electroactivated CC in practical devices.
