The use of solar energy to produce hydrogen has been one of the research hotspots in recent years.With the continuous exploitation of solar hydrogen evolution,the performance of photo(electro)catalysts has been greatl...The use of solar energy to produce hydrogen has been one of the research hotspots in recent years.With the continuous exploitation of solar hydrogen evolution,the performance of photo(electro)catalysts has been greatly optimized.However,the solar-driven hydrogen production for most semiconductors,especially for organic semiconductors,is limited due to the lack of active centers and serious electron–hole recombination.Recently,it has been reported that carbon-carbon triple bonds(C≡C)can function as active sites for hydrogen evolution,and diacetylenic moiety in organic semiconductors is able to increase carrier migration as well.Therefore,organic semiconductors containing C≡C have attracted considerable attention in the past few years.In this review,organic materials or organic–inorganic hybrids containing C≡C for photo(electro)catalytic solar hydrogen production are classified first,including graphdiyne,conjugated acetylene polymers,some covalent organic frameworks,and metal–organic frameworks.After that,the structure,properties,and advantages and disadvantages of C≡C-containing materials are introduced and summarized.Apart from these,this review also presents advances in materials containing C≡C in the field of solar hydrogen generation.Finally,perspectives on the future development of C≡C-containing materials in the field of solar hydrogen generation are also briefly anticipated.This review provides pertinent insights into the main challenges and potential advances in the organic semiconductors for solar-driven hydrogen production,which will also greatly contribute to other photo(electro)catalytic reactions.展开更多
Alzheimer's disease(AD)is a neurodegenerative disease and a major threat to human health worldwide.The association between aluminum exposure and AD has been widely reported.Owing to the ubiquitous presence of alum...Alzheimer's disease(AD)is a neurodegenerative disease and a major threat to human health worldwide.The association between aluminum exposure and AD has been widely reported.Owing to the ubiquitous presence of aluminum in daily life;aluminum exposure can easily occur whenever and wherever possible.Thus;a rapid and sensitive reagent for detecting aluminum and assist in AD daily prevention for potential AD patient population is extremely needed.However;existing aluminum detection methods rely on precise instruments;which are impractical for household use.Herein;a series of aggregation-induced emission-based covalent-organic framework(AIE-COF)fluorescent probes has been designed with progressively tuned sizes and screened for aluminum detection.Among them;COF-N2 was found to have the highest response towards aluminum specifically;with a fluorescence intensity change of 19.14 times before and after chelation;which could determine the aluminum concentration by naked eye.Then;the molecular mechanism of COF-N2 fluorescence changes was explained and COF-N2 was used for both diagnose the aluminum distribution in various organs of APP/PS1 transgenic mice and quickly determine the aluminum content in daily necessities.The use of AIE-COF probes for aluminum detection provides a promising avenue for developing aluminum related AD clinical diagnosis and daily prevention tools.展开更多
The photocatalytic activation of sulfites,a common by-product in industries,is a green and sustainable technology with great promise for the treatment of refractory pollutants in water.In this study,N vacancies and N ...The photocatalytic activation of sulfites,a common by-product in industries,is a green and sustainable technology with great promise for the treatment of refractory pollutants in water.In this study,N vacancies and N doping were constructed at precise sites in graphitic carbon nitride(CN),following the combination with biochar(BC),synthesizing the BVCN with excellent photocatalytic activation of sulfites under solar light.When the BC was 5wt%(5BVCN),the reaction rate constant of reactive red 120(RR120)in SO_(3)^(2−)-containing solution reached 0.0247 min^(-1),which was 5.49 times of CN and 15.43 times of 5BVCN in SO_(3)^(2−)-free solution.Characterizations and density functional theory(DFT)calculations revealed that N vacancies could trap electrons,while N doping regulated the electronic structure,forming mid-gap states to enhance the separation of carriers.In BVCN,BC rich in pyridinic N serves as both electron transfer channel and electron storage medium,havingπ-πinteraction with structurally regulated CN(VCN).BVCN has narrower band gap and low recombination rate of photogenerated carriers,responds well to visible light,and is easy to firmly associated with SO_(3)^(2−),enhancing the electron transfer from SO_(3)^(2−)to BVCN.In the SO_(3)^(2−)-containing system,the primary active species were identified as SO_(3)^(•−),•O_(2)^(−)and h^(+).Moreover,BVCN exhibited good stability and recyclability.The system shows potential for treating wastewater containing sulfites,realizing resource utilization.展开更多
Proteolytic degradation of amyloid-β （Aβ） aggregates and clearance of Aβ- induced reactive oxygen species （ROS） have received significant attention for the treatment of Alzheimer＇s disease （AD）. However, it ...Proteolytic degradation of amyloid-β （Aβ） aggregates and clearance of Aβ- induced reactive oxygen species （ROS） have received significant attention for the treatment of Alzheimer＇s disease （AD）. However, it is difficult, and often unfeasible, to directly upregulate or transport intraceUular native enzymes. More importantly, penetration of the blood-brain barrier （BBB） has presented a major impediment. Herein, we report on the rational design of a polyoxometalate- based nanozyme with both protease-like activity for depleting A~ aggregates, and superoxide dismutase （SOD）-like activity for scavenging A[3-mediated ROS. Furthermore, this nanozyme acts as a metal chelator to remove Cu from Cu-induced Aβ oligomers. More intriguingly, the nanozyme can cross the BBB and exhibits low toxicity. This work provides new insights into the design and synthesis of inorganic nanozymes as multifunctional therapeutic agents in the treatment of AD.展开更多
Semiconductor nanomaterials with photocatalytic activity have potential for many applications. An effective way of promoting photocatalytic activity is depositing noble metal nanoparticles （NPs） on a semiconductor, ...Semiconductor nanomaterials with photocatalytic activity have potential for many applications. An effective way of promoting photocatalytic activity is depositing noble metal nanoparticles （NPs） on a semiconductor, since the noble metal NPs act as excellent electron acceptors which inhibit the quick recombination of the photoexcited electron-hole pairs and thereby enhance the generation of reactive oxygen species （ROS）. Herein, a highly effective platform, graphitic carbon nitride （g-C3N4） nanosheets with embedded Ag nanopartides （Ag/g-C3N4）, was synthesized by a facile route. Under visible light irradiation, the ROS production of Ag/g-C3N4 nanohybrids was greatly improved compared with pristine g-C3N4 nanosheets, and moreover, the nanohybrids showed enhanced antibacterial efficacy and ability to disperse bacterial biofilms. We demonstrate for the first time that the Ag/g-C3N4 nanohybrids are efficient bactericidal agents under visible light irradiation, and can also provide a new way for biofilm elimination. The enhanced antibacterial properties and biofilm-disrupting ability of Ag/g-C3N4 nanohybrids may offer many biomedical applications.展开更多
To realize continuously and stably work in a“moist/hot environment”,flexible electronics with excellent humid resistance,antiswelling,and detection sensitivity are demanding.Herein,a solvent-resistant and temperatur...To realize continuously and stably work in a“moist/hot environment”,flexible electronics with excellent humid resistance,antiswelling,and detection sensitivity are demanding.Herein,a solvent-resistant and temperature-ultrasensitive hydrogel sensor was prepared by combining MXene and quaternized chitosan(QCS)with the binary polymer chain.The strong electrostatic interaction between the QCS chain and the poly(acrylic acid)(PAA)network endows the hydrogel stability against solvent erosion,high temperature,and high humidity.The strong dynamic interaction between MXene and polymer matrix significantly improves the mechanical properties and sensing(strain and temperature)sensitivity of the hydrogel.The hydrogel strain sensor exhibits a high gauge factor(5.53),temperature/humidity tolerance(equilibrium swelling ratio of 2.5%at 80℃),and excellent cycle stability,which could achieve a remote and accurate perception of complex human motion and environment fluctuation under aquatic conditions.Moreover,the hydrogel sensor exhibits impressive thermal response sensitivity(-3.183%/℃),ultrashort response time(<2.53 s),and a low detection limit(<0.5℃)in a wide temperature range,which is applied as an indicator of the body surface and ambient temperature.In short,this study broadens the application scenarios of hydrogels in persistent extreme thermal and wet environments.展开更多
基金The authors are grateful for the financial support from theNational Natural Science Foundation of China(22209076,22232004,22279062)the National Key Research andDevelopment Program of China(2021YFA1502700)the Natural Science Foundation of Jiangsu Province (GrantNo.BK 20220369)
文摘The use of solar energy to produce hydrogen has been one of the research hotspots in recent years.With the continuous exploitation of solar hydrogen evolution,the performance of photo(electro)catalysts has been greatly optimized.However,the solar-driven hydrogen production for most semiconductors,especially for organic semiconductors,is limited due to the lack of active centers and serious electron–hole recombination.Recently,it has been reported that carbon-carbon triple bonds(C≡C)can function as active sites for hydrogen evolution,and diacetylenic moiety in organic semiconductors is able to increase carrier migration as well.Therefore,organic semiconductors containing C≡C have attracted considerable attention in the past few years.In this review,organic materials or organic–inorganic hybrids containing C≡C for photo(electro)catalytic solar hydrogen production are classified first,including graphdiyne,conjugated acetylene polymers,some covalent organic frameworks,and metal–organic frameworks.After that,the structure,properties,and advantages and disadvantages of C≡C-containing materials are introduced and summarized.Apart from these,this review also presents advances in materials containing C≡C in the field of solar hydrogen generation.Finally,perspectives on the future development of C≡C-containing materials in the field of solar hydrogen generation are also briefly anticipated.This review provides pertinent insights into the main challenges and potential advances in the organic semiconductors for solar-driven hydrogen production,which will also greatly contribute to other photo(electro)catalytic reactions.
基金supported by the National Key R&D Program of China(2022YFB3805902)the National Natural Science Foundation of China(22131004,U21A20330,21975039 and 22077118)+3 种基金the“111”project(B18012)the Fundamental Research Funds for the Central Universities,Excellent Youth Team Program(2412023YQ001)the Finance Special Project on Medical and Health Talents of the Finance Department of Jilin Province(JLSWSRCZX2023-52)WBE Liver Fibrosis Foundation(2020009).
文摘Alzheimer's disease(AD)is a neurodegenerative disease and a major threat to human health worldwide.The association between aluminum exposure and AD has been widely reported.Owing to the ubiquitous presence of aluminum in daily life;aluminum exposure can easily occur whenever and wherever possible.Thus;a rapid and sensitive reagent for detecting aluminum and assist in AD daily prevention for potential AD patient population is extremely needed.However;existing aluminum detection methods rely on precise instruments;which are impractical for household use.Herein;a series of aggregation-induced emission-based covalent-organic framework(AIE-COF)fluorescent probes has been designed with progressively tuned sizes and screened for aluminum detection.Among them;COF-N2 was found to have the highest response towards aluminum specifically;with a fluorescence intensity change of 19.14 times before and after chelation;which could determine the aluminum concentration by naked eye.Then;the molecular mechanism of COF-N2 fluorescence changes was explained and COF-N2 was used for both diagnose the aluminum distribution in various organs of APP/PS1 transgenic mice and quickly determine the aluminum content in daily necessities.The use of AIE-COF probes for aluminum detection provides a promising avenue for developing aluminum related AD clinical diagnosis and daily prevention tools.
基金support from the National Natural Science Foundation of China(Grant No.52170073)the Outstanding Youth Science Foundation of Heilongjiang Province,China(Grant No.YXQQ2440402223).
文摘The photocatalytic activation of sulfites,a common by-product in industries,is a green and sustainable technology with great promise for the treatment of refractory pollutants in water.In this study,N vacancies and N doping were constructed at precise sites in graphitic carbon nitride(CN),following the combination with biochar(BC),synthesizing the BVCN with excellent photocatalytic activation of sulfites under solar light.When the BC was 5wt%(5BVCN),the reaction rate constant of reactive red 120(RR120)in SO_(3)^(2−)-containing solution reached 0.0247 min^(-1),which was 5.49 times of CN and 15.43 times of 5BVCN in SO_(3)^(2−)-free solution.Characterizations and density functional theory(DFT)calculations revealed that N vacancies could trap electrons,while N doping regulated the electronic structure,forming mid-gap states to enhance the separation of carriers.In BVCN,BC rich in pyridinic N serves as both electron transfer channel and electron storage medium,havingπ-πinteraction with structurally regulated CN(VCN).BVCN has narrower band gap and low recombination rate of photogenerated carriers,responds well to visible light,and is easy to firmly associated with SO_(3)^(2−),enhancing the electron transfer from SO_(3)^(2−)to BVCN.In the SO_(3)^(2−)-containing system,the primary active species were identified as SO_(3)^(•−),•O_(2)^(−)and h^(+).Moreover,BVCN exhibited good stability and recyclability.The system shows potential for treating wastewater containing sulfites,realizing resource utilization.
基金Financial support was provided by the National Basic Research Program of China （973 Project） （Nos. 2011CB936004 and 2012CB720602） and the National Natural Science Foundation of China （Nos. 21210002, 21431007, 21402183, and 21533008）.
文摘Proteolytic degradation of amyloid-β （Aβ） aggregates and clearance of Aβ- induced reactive oxygen species （ROS） have received significant attention for the treatment of Alzheimer＇s disease （AD）. However, it is difficult, and often unfeasible, to directly upregulate or transport intraceUular native enzymes. More importantly, penetration of the blood-brain barrier （BBB） has presented a major impediment. Herein, we report on the rational design of a polyoxometalate- based nanozyme with both protease-like activity for depleting A~ aggregates, and superoxide dismutase （SOD）-like activity for scavenging A[3-mediated ROS. Furthermore, this nanozyme acts as a metal chelator to remove Cu from Cu-induced Aβ oligomers. More intriguingly, the nanozyme can cross the BBB and exhibits low toxicity. This work provides new insights into the design and synthesis of inorganic nanozymes as multifunctional therapeutic agents in the treatment of AD.
基金This work was supported by the National Basic Research Program of China （Nos. 2011CB936004 and 2012CB720602） and the National Natural Science Foundation of China （Nos. 21210002, 21431007, 91413111, 21402183）.
文摘Semiconductor nanomaterials with photocatalytic activity have potential for many applications. An effective way of promoting photocatalytic activity is depositing noble metal nanoparticles （NPs） on a semiconductor, since the noble metal NPs act as excellent electron acceptors which inhibit the quick recombination of the photoexcited electron-hole pairs and thereby enhance the generation of reactive oxygen species （ROS）. Herein, a highly effective platform, graphitic carbon nitride （g-C3N4） nanosheets with embedded Ag nanopartides （Ag/g-C3N4）, was synthesized by a facile route. Under visible light irradiation, the ROS production of Ag/g-C3N4 nanohybrids was greatly improved compared with pristine g-C3N4 nanosheets, and moreover, the nanohybrids showed enhanced antibacterial efficacy and ability to disperse bacterial biofilms. We demonstrate for the first time that the Ag/g-C3N4 nanohybrids are efficient bactericidal agents under visible light irradiation, and can also provide a new way for biofilm elimination. The enhanced antibacterial properties and biofilm-disrupting ability of Ag/g-C3N4 nanohybrids may offer many biomedical applications.
基金The work was supported by the National Key R&D Program of China(No.2020YFA0709900)“Taishan scholars”construction special fund of Shandong Province。
文摘To realize continuously and stably work in a“moist/hot environment”,flexible electronics with excellent humid resistance,antiswelling,and detection sensitivity are demanding.Herein,a solvent-resistant and temperature-ultrasensitive hydrogel sensor was prepared by combining MXene and quaternized chitosan(QCS)with the binary polymer chain.The strong electrostatic interaction between the QCS chain and the poly(acrylic acid)(PAA)network endows the hydrogel stability against solvent erosion,high temperature,and high humidity.The strong dynamic interaction between MXene and polymer matrix significantly improves the mechanical properties and sensing(strain and temperature)sensitivity of the hydrogel.The hydrogel strain sensor exhibits a high gauge factor(5.53),temperature/humidity tolerance(equilibrium swelling ratio of 2.5%at 80℃),and excellent cycle stability,which could achieve a remote and accurate perception of complex human motion and environment fluctuation under aquatic conditions.Moreover,the hydrogel sensor exhibits impressive thermal response sensitivity(-3.183%/℃),ultrashort response time(<2.53 s),and a low detection limit(<0.5℃)in a wide temperature range,which is applied as an indicator of the body surface and ambient temperature.In short,this study broadens the application scenarios of hydrogels in persistent extreme thermal and wet environments.
