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An ultra-porous g-C_(3)n_(4) micro-tube coupled with MXene(Ti_(3)C_(2)TX)nanosheets for efficient degradation of organics under natural sunlight

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Journal of Environmental Sciences 2024年第3期137卷 258-270页

作者： Zongyang Ya Qiyou Wang Jingjin cai Peng Wang Xinyu Jiang Zhiyin cai Shanglin Xiang Tingwei Wang Dongyu cai College of Materials Science&Engineering Nanjing Tech University30 South PuZhu RoadNanjing 211816China Key Laboratory of Flexible Electronics(KLOFE)&Institute of Advanced Materials(IAM) Jiangsu National Synergetic Innovation Center for Advanced Materials(SICAM)Nanjing Tech University30 South PuZhu RoadNanjing 211816China

It remains as a challenge for realizing efficient photo-responsive catalysts towards largescale degradation of organic pollutants under natural *** work reports a new pore engineering strategy for creating ultra-porous g-C_(3)n_(4) micro-tubes with an unprecedentedly high specific surface area of 152.96 m^(2)/*** is mainly associated with releasing internal vapor pressure in the autoclave where the hydrothermal treatment of the urea/melamine mixture is *** by microscopic observation,porosity measurement and spectroscopic characterization,it is found that releasing the pressure at halfway of hydrothermal process is vital for forming exfoliated rod-like precursors and the de-aggregation of these rods presents substantial benefits on the production of mesopores on g-C_(3)n_(4) microtubes during the calcination of *** offers a large number of reactive sites required by photocatalytic *** these micro-tubes with Ti_(3)C_(2)T_(X) nanosheets via electrostatic interaction yields a 1D/2D heterojunction with a close interfacial *** addition of metallically conductive Ti_(3)C_(2)T_(X) nanosheets accelerates the separation between electrons and holes,and also enhances the light *** these merits of structural design lead to forming a group of highly efficient catalysts demonstrating an excellent photocatalytic degradation rate of k=0.0560 min^(-1)for RhB dyes under 100 mW/cm~2 visible light radiation that micks sunlight *** laboratory valuation is further supported by an outdoor test that shows a fast degradation rate of 0.0744 min^(-1)under natural sunlight.

关键词： Carbon nitride MXene Heterojunction Photocatalysis

n-Heterocyclic carbene-catalyzed enantioselective(dynamic) kinetic resolutions and desymmetrizations

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Science China Chemistry 2024年第2期67卷 482-511页

作者： Yi Zhang Hui cai Xiuhai Gan Zhichao Jin national Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide and Agricultural BioengineeringMinistry of EducationGuizhou UniversityHuaxi DistrictGuiyang550025China

n-heterocyclic carbene-catalyzed enantioselective kinetic resolutions,dynamic kinetic resolutions,and desymmetrization reactions are systematically *** content is organized according to the activation modes involved i... 详细信息

关键词： n-heterocyclic carbene kinetic resolution dynamic kinetic resolution desymmetrization organocatalysis

Impact of COVID-19 on the energy consumption of commercial buildings:A case study in Singapore

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Energy and Built Environment 2024年第3期5卷 364-373页

作者： Senhong cai Zhonghua Gou School of Urban Design Wuhan UniversityWuhanChina

numerous studies have demonstrated that commercial activities have significantly reduced during COVID-19,while there are few studies disclosing the consequent impacts on the energy consumption of commercial *** study explores the changes in energy consumption of different types of commercial buildings in Sin-gapore under the impact of the pandemic,using commercial building energy performance data from 2017 to 2020(n=540).The sampled buildings include 93 hotel buildings,303 office buildings,106 retail buildings,and 38 mixed *** analysis mainly used linear regression and paired sample *** results showed that relative to 2019,the mean energy use intensity(EUI)of sampled commercial buildings decreased by 56.77 kWh/m^(2)in the pandemic year(2020),a plunge of 19.9%.The extent to which the EUI of each type of commercial building is affected by the pandemic is found as:mixed development>retail>office>*** study also identi-fied the factors that significantly influenced the EUI of commercial buildings before and during the *** results of the study complement existing knowledge about the factors influencing energy consumption in com-mercial buildings by considering the impact of the pandemic and furthermore contribute to the improvement of energy management in commercial buildings by providing directions for building energy efficiency approaches.

关键词： Commercial buildings Energy consumption Energy use intensity Impact of COVID-19 Influential factors

A single atom photocatalyst co-doped with potassium and gallium for enhancing photocatalytic hydrogen peroxide synthesis

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nano Research 2024年第8期17卷 7027-7038页

作者： Wenan cai Yuichiro Tanaka Xing Zhu Teruhisa Ohno Department of Applied Chemistry Faculty of EngineeringKyushu Institute of TechnologyKitakyushu 804-8550Japan College of Bioresources Chemical and Materials Engineering Shaanxi University of Science&TechnologyXi’an 710021China

Polymer carbon nitride(PCn)is widely used in ***,pristine PCn has disadvantages such as insufficient visible light absorption and low photogenerated carrier separation efficiency that greatly limited the photocatalytic *** a non-toxic metal,gallium has the potential to solve the defects of *** ions coordinated with nitrogen in carbon nitride to form Ga-n active sites and improved the photocatalytic *** doped potassium ions form a transmission channel for charge redistribution and transfer between adjacent layers,which is beneficial for better separation of photoexcited *** this study,a series of PCn co-doped with gallium and potassium(Ga-K-PCn)were *** experimental results indicated photocatalytic generation of hydrogen peroxide proceeds through the 2e−oxygen reduction reaction ***,nyquist plots and photocurrent results further proved that the presence of Ga-n sites and potassium ion doping could significantly improve the separation/transfer of intra-planar and interlayer charge carriers and thus enhance photocatalytic *** Ga10-K3-PCn photocatalysts promoted yield of H_(2)O_(2),with reactivity at 28.2μmol/(g·h)and solar-to-chemical conversion efficiency at 0.64%,surpassed that of a typical photo-catalyst based on PCn(0.18%).

关键词： photocatalysis gallium oxygen reduction reaction H_(2)O_(2) production

Graphitic carbon nitride nanosheets mitigate cadmium toxicity in Glycine max *** promoting cadmium retention in root and improving photosynthetic performance

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Journal of Environmental Sciences 2024年第5期139卷 543-555页

作者： Kai Xu Yunyu Guo Chenghua Xing Ronglong Fu Bin Zou Rongchuan Liu Luyi cai Jianfang Yan Xi-Lin Wu Miaozhen cai College of Geography and Environmental Sciences Zhejiang Normal UniversityJinhua 321004China College of Agriculture Jinhua PolytechnicJinhua 321007China

Cadmium(Cd)pollution poses a serious threat to plant growth and *** have shown great application potential for alleviation of Cd toxicity to *** this study,we applied graphitic carbon nitride nanosheets(g-C_(3)n_(4)nSs)for alleviation of Cd-toxicity to soybean(Glycine max L.).The g-C_(3)n_(4)nSs supplementation significantly improved plant growth and reduced oxidative damage in the Cd-toxicated soybean seedlings through hydroponic ***,the g-C_(3)n_(4)nSs dynamically regulated the root cell wall(RCW)components by increasing pectin content and modifying its demethylation via enhancing pectin methylesterase(PME)activity,therefore greatly enhanced stronger RCW-Cd retention(up to 82.8%)and reduced Cd migration to the ***,the g-C_(3)n_(4)nSs reversed the Cd-induced chlorosis,increased photosynthetic efficiency because of enhancement in F_v/F_mration,Y(Ⅱ)and sugars *** results provide new insights into the alleviation of Cd toxicity to plants by g-C_(3)n_(4)nSs,and shed light on the application of low-cost and environmental-friendly carbon-based nMs for alleviating heavy metal toxicity to plants.

关键词： Cadmium Carbon nitride nanosheets Cell wall Pectin Pectin methylesterase Soybean

Tailoring sulfur-doped and nitrogen-defective carbon nitride nanosheets for efficient photo-controlled radical polymerizations

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Science China Chemistry 2024年第7期67卷 2325-2334页

作者： Xue Li Meng Kai Xu Yuan Huang Tao cai Key Laboratory of Biomedical Polymers of Ministry of Education College of Chemistry and Molecular SciencesWuhan UniversityWuhan 430072China Wuhan University Shenzhen Research Institute Shenzhen 518057China

Despite the challenges that remain,the synergistic adjustment of various microstructures and photochemical parameters of graphitic carbon nitride(g-C_(3)n_(4))in photocatalytic reactions holds promises for improving catalytic efficiency and reducing energy ***,sulfur-doped and nitrogen-defective g-C_(3)n_(4)(n-SC_(3)n_(x))nanosheets were designed and elaborately *** resultant n-SC_(3)n_(x)possessed a precisely defined 2D layer structure with extensive porosity and incremental specific surface *** photoinduced electron transfer-reversible addition-fragmentation chain transfer(PET-RAFT)polymerization of vinyl monomers with low dispersity,excellent temporal control and high chain-end fidelity was achieved under mild blue light irradiation in a nondegassed *** to their ultrathin nanostructures with nitrogen defects and sulfur dopants,n-SC_(3)n_(x)was capable of catalyzing RAFT polymerization in aqueous solutions at significantly accelerated rates,which were nearly 8 times faster compared to bulk g-C_(3)n_(4).The ease of separation and efficient reusability in subsequent polymerizations was enabled by the heterogeneous nature of n-SC_(3)n_(x).The appeal of this approach was illustrated by the fact that utilizing a reusable and metal-free photocatalyst in aqueous environments allowed for the synthesis of polymers with molecular weight up to 300 kg mol^(-1) and a dispersity of 1.32.

关键词： graphitic carbon nitride nitrogen defects sulfur dopants PET-RAFT polymerization recyclability

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Upgrading waste nO_(x) into amino acids via electrocatalysis on Co nanoparticles encapsulated in hollow carbon nanofibers

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Science China Chemistry 2024年第6期67卷 1946-1952页

作者： Jiahui Xian Kaixing cai Peisen Liao Shihan Wang Guangqin Li Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFMIGCMESchool of ChemistrySun Yat-Sen UniversityGuangzhou510275China

Electrocatalytic conversion of waste nitrogen oxide(nO_(x))into value-added nitrogenous chemicals,especially amino acid,is an emerging strategy to alleviate nO_(x)***,this process suffers from the coexistence of multiple competitive reactions leading to complex product distribution and low efficiency,and thus the rational design and modulation of efficient catalysts remains a formidable ***,well-designed Co nanoparticles encapsulated in hollow carbon nanofiber(CoHCnF)were constructed to promote the amino acid electrosynthesis via dealing waste nO_(x)coupling with biomass-derived keto *** to the rapid reactant diffusion,electron transport and efficient contact with abundant accessible Co catalytic sites stemmed from the unique hollow nanotubular structure,Co-HCnF manifested impressive glycine synthesis performance in one-pot adopting nO as the nitrogen source with Faradaic efficiency(FE)of 41.7%and a corresponding yield rate of 222.3μmol h^(-1)as well as 120 h robust ***,it also demonstrates an excellent performance with the FE of 42.8%for nO_(3)~-solution as the nitrogen ***,this strategy displays a broad universality for the synthesis of other amino *** work not only highlights the importance of hollow-structuring electrocatalyst towards upgrading wasted nO_(x)species into amino acids,but also promotes the further development of electrosynthetic systems for high-valued n-containing organic chemicals.

关键词： electrocatalysis nO_(x)reduction amino acid porous materials hollow structure

Facile intercalation of alkali ions in WO_(3)for modulated electronic and optical properties:Implications for artificial synapses and chromogenic application

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Science China(Physics,Mechanics & Astronomy) 2024年第2期67卷 149-160页

作者： Changmeng Huan Zihan Lu Silin Tang Yongqing cai Qingqing Ke School of Microelectronics Science and Technology Sun Yat-sen UniversityZhuhai 519082China Guangdong Provincial Key Laboratory of Optoelectronic Information Processing Chips and Systems Sun Yat-sen UniversityZhuhai 519082China Institute of Applied Physics and Materials Engineering University of MacaoTaipaMacao 999078China

Tungsten oxides(WO_(3))are widely recognized as multifunctional systems owing to the existence of rich *** diverse phases exhibit distinct octahedra-tilting patterns,generating substantial tunnels that are ideally suited for ***,a quantitative comprehension regarding the impact of distinct phases on the kinetics of intercalated conducting ions remains ***,we employ first-principles calculations to explore the spatial and orientational correlations of ion transport inγ-and h-WO_(3),shedding light on the relationship between diffusion barriers and the size of the conducting *** findings reveal that different types and concentrations of alkali-metals induce distinct and continuous lattice distortions in WO_(3)***,γ-WO_(3)is more appropriate to accommodate Li+ions,exhibiting a diffusion barrier and coefficient of 0.25 eV and 9.31×10^(-8)cm^(2)s^(-1),***,h-WO_(3)features unidirectional and sizeable tunnels that facilitate the transport of K+ions with an even lower barrier and a high coefficient of 0.11 e V and 2.12×10^(-5)cm^(2)s^(-1),***,the introduction of alkali-metal into WO_(3)tunnels tends to introduce n-type conductivity by contributing s-electrons to the unoccupied W 5d states,resulting in enhanced conductivity and tunable electronic *** alkali metals in WO_(3)tunnels are prone to charge transfer,forming small polaronic states and modulating the light absorption in the visible and nearinfrared *** tunable electronic and optical properties,combined with the high diffusion coefficient,underscore the potential of WO_(3)in applications such as artificial synapses and chromogenic devices.

关键词： WO_(3)polymorphs ion insertion kinetic activity tunable electronic and optical properties iontronics

In situ embedded bismuth nanoparticles among highly porous carbon fibers for efficient carbon dioxide reduction

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Rare Metals 2024年第9期43卷 4312-4320页

作者： Wei-Jian Guo Ao Zhou Wen-Wen cai Jin-Tao Zhang Key Laboratory for Colloid and Interface Chemistry (Ministry of Education) School of Chemistry and Chemical EngineeringShandong University

Electrocatalysis provides an optimal approach for the conversion of carbon dioxide(CO2) into high-value chemicals, thereby presenting a promising avenue toward achieve carbon neutrality. However, addressing the selectivity and stability challenges of metal catalysts in electrolytic reduction remains a daunting task. In this study, the electrospinning method is employed to fabricate porous carbon nanofibers loaded with bismuth nanoparticles with the help of in situ pyrolysis. The porous carbon nanofibers as conductive support would facilitate the dispersion of bismuth active sites while inhibiting their aggregation and promoting the mass transfer, thus enhancing their electrocatalytic activity and stability. Additionally, nitrogen doping induces electron delocalization in bismuth atoms through metal-support interactions, thus enabling efficient adsorption of intermediates for improving selectivity based on the theoretical calculation. Consequently, Bi@PCnF-500 exhibits the exceptional selectivity and stability across a wide range of potential windows. notably, its faradaic efficiency(FE) of formate reaches 92.7% in H-cell and94.9% in flow cell, respectively, with good electrocatalytic stability. The in situ characterization and theoretical calculations elucidate the plausible reaction mechanism to obtain basic rules for designing efficient electrocatalyst.

关键词： Carbon dioxide reduction Electron delocalization n-doping Porous carbon nanofiber