Photosynthesis of H_(2)O_(2)via sustainable biomass-derived carbon catalysts facilitate the conversion of renewable resources into valuable chemicals.However,the regulatory function of surface functional groups over r...Photosynthesis of H_(2)O_(2)via sustainable biomass-derived carbon catalysts facilitate the conversion of renewable resources into valuable chemicals.However,the regulatory function of surface functional groups over reaction kinetics has not been sufficiently investigated.Herein,hydrothermal carbon spheres(CS)rich in oxygencontaining functional groups demonstrated a remarkably high H_(2)O_(2)production rate(653μmol/(g·h))in both pure water and actual seawater,even in the absence of any sacrificial agent.Meanwhile,the catalyst demonstrates outstanding activity(92%conversion and>99%selectivity)in the visible-light-driven photocatalytic oxidation of benzylamine to imines.Comprehensive analysis reveals that CS was rich in surface oxygen-containing functional groups,a feature strongly associated with its high photocatalytic efficiency.The observed positive Zeta potential of CS in seawater likely diminished the electrostatic repulsion against the positively charged intermediates,thereby facilitating their accumulation at the liquid-solid interface.This work proposes a strategic framework for developing metal-free photocatalysts from biomass,offering a sustainable pathway for photocatalytic applications.展开更多
The metal‐reduction‐induced dechlorination coupling(MR-DC)strategy enables the first successful synthesis of an all‐inorganic crosslinked phosphazene network(aPN)from hexachlorocyclotriphosphazene(HCCP)under mild r...The metal‐reduction‐induced dechlorination coupling(MR-DC)strategy enables the first successful synthesis of an all‐inorganic crosslinked phosphazene network(aPN)from hexachlorocyclotriphosphazene(HCCP)under mild reaction conditions.Using Cu as a model,the resulting Cu-aPN(copper‐embedded all‐inorganic phosphazene network)retains the intrinsic N_(3)P_(3)backbone and exhibits an amorphous structure where Cu species are uniformly anchored at dense P/N coordination sites of the network.Time of flight secondary ion mass spectrometry(TOF‐SIMS)and X‐ray diffraction(XRD)reveal a gradual CuCl‐to‐CuO phase conversion during ammonia treatment,which effectively ensures the structural stability of the phosphazene framework.In 1 M KOH,Cu-aPN delivers an overpotential of 280 mV at 10 mA cm^(−2)and a Tafel slope of 48 mV dec^(−1),markedly outperforming Ga-aPN.In situ Raman and density functional theory(DFT)analyses indicate stronger Cu-P/N coordination coupling that lowers the*OH formation barrier(0.39 vs.0.88 eV for Ga).This MR-DC route furnishes a general and versatile pathway for constructing metal‐embedded all‐inorganic phosphazene frameworks with tunable coordination environments for advanced electrocatalytic applications.展开更多
Dendritic spines are small protrusions along dendrites that contain most of the excitatory synapses in principal neurons,playing a crucial role in neuronal function by creating a compartmentalized environment for sign...Dendritic spines are small protrusions along dendrites that contain most of the excitatory synapses in principal neurons,playing a crucial role in neuronal function by creating a compartmentalized environment for signal transduction.The plasticity of spine morphologies provides a tunable handle to regulate calcium signal dynamics,allowing rapid regulation of protein expression necessary to establish and maintain synapses(Cornejo et al.,2022).If excitatory inputs were to be located primarily on dendritic shafts,dendrites would frequently short-circuit,preventing voltage signals from propagating(Cornejo et al.,2022).It is thus not surprising that the structural plasticity of dendritic spines is closely linked to synaptic plasticity and memory formation(Berry and Nedivi,2017).While comprehensive in vitro studies have been conducted,in vivo studies that directly tackle the mechanism of dendritic transport and translation in regulating spine plasticity spatiotemporally are limited.展开更多
Microorganisms can colonize the surface of microplastics(MPs)to form a distinctive microbiome,known as a“plastisphere”which is regarded as an anthropogenic niche for microbial growth.However,bacterial community asse...Microorganisms can colonize the surface of microplastics(MPs)to form a distinctive microbiome,known as a“plastisphere”which is regarded as an anthropogenic niche for microbial growth.However,bacterial community assembly in virgin and aging MP plastispheres across different habitats is poorly understood.This study aims to assess the variations in bacterial community assembly across different niches and habitats with an in situ ex-periment,in which constructed forest wetland(FW),natural lake wetland(LW),and lotus pond wetland(LP)were habitats,and plastispheres of virgin and aging low-density polyethylene(LDPE)MPs,as well as surround-ing wetland soils were niches.Significant niche-related differences in bacterial communities were observed,with lower diversity and enrichment of potential plastic-degrading bacteria in the plastisphere than in the soil bacterial communities.Furthermore,habitat-related differences exerted a more pronounced influence on the beta-diversity patterns of the bacterial communities.The linear regression analyses indicated that the local species pool con-tributed more to bacterial community assembly in the LW wetland,whereas the relative abundance of species was the primary factor in the LP wetland.The null model analysis indicated that plastisphere bacterial communi-ties were predominantly driven by the stochastic process,with a more deterministic assembly observed in the LP wetland and soil bacterial communities.Additionally,the primary ecological process shaping plastisphere com-munities shifted from drift in the virgin LDPE to homogenising dispersal in the aging LDPE.This study provides new insights into the fate and ecological impacts of MPs in wetlands,thereby facilitating the effective regulations of plastic pollution.展开更多
Violet phosphorus,a recently explored layered elemental semiconductor,has attracted much attention due to its unique photoelectric,mechanical properties,and high hole mobility.Herein,violet arsenic phosphorus has for ...Violet phosphorus,a recently explored layered elemental semiconductor,has attracted much attention due to its unique photoelectric,mechanical properties,and high hole mobility.Herein,violet arsenic phosphorus has for the first time been synthesized by a molten lead method.The crystal structure of violet arsenic phosphorus(P^(83.4)As_(0.6),CSD-2408761)was determined by single crystal X-ray diffraction to have similar structure as that of violet phosphorus,where P12 is occupied by arsenic/phosphorus(As/P)atoms as mixed occupancy sites As1/P12.The arsenic substitution has been demonstrated to tune the band structure of violet phosphorus,switching p-type of violet phosphorus to high-performance n-type violet arsenic phosphorus.The effective electron mass along the<010>direction is significantly reduced from 1.792 to 0.515 m_(0)by arsenic substitution,resulting in an extremely high electron mobility of 2622.503 cm^(2)V^(-1)s^(-1).The field effect transistor built with P_(83.4)As_(0.6)nanosheets was measured to have a high electron mobility(137.06 cm^(2)V^(-1)s^(-1),61.2 nm),even under ambient conditions for 5 h,much higher than the hole mobility of violet phosphorene nanosheets(4.07 cm^(2)V^(-1)s^(-1),73.3 nm).This work provides a new idea for designing phosphorus-based materials for field effect transistors,giving significant potential in complementary metal-oxide-semiconductor applications.展开更多
基金Supported by the Natural Science Foundation of Shanxi Province(202203021222233,202203021212398,202203021212403)。
文摘Photosynthesis of H_(2)O_(2)via sustainable biomass-derived carbon catalysts facilitate the conversion of renewable resources into valuable chemicals.However,the regulatory function of surface functional groups over reaction kinetics has not been sufficiently investigated.Herein,hydrothermal carbon spheres(CS)rich in oxygencontaining functional groups demonstrated a remarkably high H_(2)O_(2)production rate(653μmol/(g·h))in both pure water and actual seawater,even in the absence of any sacrificial agent.Meanwhile,the catalyst demonstrates outstanding activity(92%conversion and>99%selectivity)in the visible-light-driven photocatalytic oxidation of benzylamine to imines.Comprehensive analysis reveals that CS was rich in surface oxygen-containing functional groups,a feature strongly associated with its high photocatalytic efficiency.The observed positive Zeta potential of CS in seawater likely diminished the electrostatic repulsion against the positively charged intermediates,thereby facilitating their accumulation at the liquid-solid interface.This work proposes a strategic framework for developing metal-free photocatalysts from biomass,offering a sustainable pathway for photocatalytic applications.
基金financially supported by the National Natural Science Foundation of China(Grant 22205173)the Innovation Capability Support Program of Shaanxi(Grant 2024CX‐GXPT‐12)。
文摘The metal‐reduction‐induced dechlorination coupling(MR-DC)strategy enables the first successful synthesis of an all‐inorganic crosslinked phosphazene network(aPN)from hexachlorocyclotriphosphazene(HCCP)under mild reaction conditions.Using Cu as a model,the resulting Cu-aPN(copper‐embedded all‐inorganic phosphazene network)retains the intrinsic N_(3)P_(3)backbone and exhibits an amorphous structure where Cu species are uniformly anchored at dense P/N coordination sites of the network.Time of flight secondary ion mass spectrometry(TOF‐SIMS)and X‐ray diffraction(XRD)reveal a gradual CuCl‐to‐CuO phase conversion during ammonia treatment,which effectively ensures the structural stability of the phosphazene framework.In 1 M KOH,Cu-aPN delivers an overpotential of 280 mV at 10 mA cm^(−2)and a Tafel slope of 48 mV dec^(−1),markedly outperforming Ga-aPN.In situ Raman and density functional theory(DFT)analyses indicate stronger Cu-P/N coordination coupling that lowers the*OH formation barrier(0.39 vs.0.88 eV for Ga).This MR-DC route furnishes a general and versatile pathway for constructing metal‐embedded all‐inorganic phosphazene frameworks with tunable coordination environments for advanced electrocatalytic applications.
基金supported by the National Natural Science Foundation of China(NSFC/RGC/JRF N_HKU735/21)Research Grant Council of Hong Kong,China(17102120,17108821,17103922,C1024-22GF,C7074-21G)+1 种基金Health and Medical Research Fund(HMRF 09200966)(to CSWL)FRQS Postdoctoral Fellowship(to AHKF).
文摘Dendritic spines are small protrusions along dendrites that contain most of the excitatory synapses in principal neurons,playing a crucial role in neuronal function by creating a compartmentalized environment for signal transduction.The plasticity of spine morphologies provides a tunable handle to regulate calcium signal dynamics,allowing rapid regulation of protein expression necessary to establish and maintain synapses(Cornejo et al.,2022).If excitatory inputs were to be located primarily on dendritic shafts,dendrites would frequently short-circuit,preventing voltage signals from propagating(Cornejo et al.,2022).It is thus not surprising that the structural plasticity of dendritic spines is closely linked to synaptic plasticity and memory formation(Berry and Nedivi,2017).While comprehensive in vitro studies have been conducted,in vivo studies that directly tackle the mechanism of dendritic transport and translation in regulating spine plasticity spatiotemporally are limited.
基金supported by Shanghai Municipal Natural Science Foundation,China(No.21ZR1446800)the National Natural Science Foundation of China(No.41877425)the Fundamental Research Funds for the Central Universities(No.226-2024-00052)。
文摘Microorganisms can colonize the surface of microplastics(MPs)to form a distinctive microbiome,known as a“plastisphere”which is regarded as an anthropogenic niche for microbial growth.However,bacterial community assembly in virgin and aging MP plastispheres across different habitats is poorly understood.This study aims to assess the variations in bacterial community assembly across different niches and habitats with an in situ ex-periment,in which constructed forest wetland(FW),natural lake wetland(LW),and lotus pond wetland(LP)were habitats,and plastispheres of virgin and aging low-density polyethylene(LDPE)MPs,as well as surround-ing wetland soils were niches.Significant niche-related differences in bacterial communities were observed,with lower diversity and enrichment of potential plastic-degrading bacteria in the plastisphere than in the soil bacterial communities.Furthermore,habitat-related differences exerted a more pronounced influence on the beta-diversity patterns of the bacterial communities.The linear regression analyses indicated that the local species pool con-tributed more to bacterial community assembly in the LW wetland,whereas the relative abundance of species was the primary factor in the LP wetland.The null model analysis indicated that plastisphere bacterial communi-ties were predominantly driven by the stochastic process,with a more deterministic assembly observed in the LP wetland and soil bacterial communities.Additionally,the primary ecological process shaping plastisphere com-munities shifted from drift in the virgin LDPE to homogenising dispersal in the aging LDPE.This study provides new insights into the fate and ecological impacts of MPs in wetlands,thereby facilitating the effective regulations of plastic pollution.
基金supported by the National Natural Science Foundation of China(Grant No.22175136)the State Key Laboratory of Electrical Insulation and Power Equipment(Grant No.EIPE23127)the Fundamental Research Funds for the Central Universities(xtr052024009,xtr052025002).
文摘Violet phosphorus,a recently explored layered elemental semiconductor,has attracted much attention due to its unique photoelectric,mechanical properties,and high hole mobility.Herein,violet arsenic phosphorus has for the first time been synthesized by a molten lead method.The crystal structure of violet arsenic phosphorus(P^(83.4)As_(0.6),CSD-2408761)was determined by single crystal X-ray diffraction to have similar structure as that of violet phosphorus,where P12 is occupied by arsenic/phosphorus(As/P)atoms as mixed occupancy sites As1/P12.The arsenic substitution has been demonstrated to tune the band structure of violet phosphorus,switching p-type of violet phosphorus to high-performance n-type violet arsenic phosphorus.The effective electron mass along the<010>direction is significantly reduced from 1.792 to 0.515 m_(0)by arsenic substitution,resulting in an extremely high electron mobility of 2622.503 cm^(2)V^(-1)s^(-1).The field effect transistor built with P_(83.4)As_(0.6)nanosheets was measured to have a high electron mobility(137.06 cm^(2)V^(-1)s^(-1),61.2 nm),even under ambient conditions for 5 h,much higher than the hole mobility of violet phosphorene nanosheets(4.07 cm^(2)V^(-1)s^(-1),73.3 nm).This work provides a new idea for designing phosphorus-based materials for field effect transistors,giving significant potential in complementary metal-oxide-semiconductor applications.
