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Single transition-metal atoms anchored on a novel Diracdispersiveπ-πconjugated holey graphitic carbon nitride substrate:computational screening toward efficient bifunctional OER/ORR electrocatalysts

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Rare Metals 2024年第8期43卷 3819-3832页

作者： Chun-Yao Fang Xi-Hang Zhang Qiang Zhang Di Liu Xiao-Meng Cui Jing-Cheng Xu Cheng-Long Shi Meng-Yu Yang college of science University of Shanghai for Science and TechnologyShanghai 200093China School of Materials and chemistry University of Shanghai for Science and TechnologyShanghai 200093China

Nonprecious-metal-group single-metal-atom catalysts with bifunctional catalytic capabilities toward the oxygen evolution reaction(OER)and oxygen reduction reaction(ORR)are highly sought after in energy-conversion and storage ***,producing renewable and sustainable energy sources remains ***,single-transition metal atoms anchored onπ-πconjugated two-dimensional(2D)graphitic carbon nitride substrates formπ-d conjugated conductive channels that enhance the overall electrocatalytic ***,firstprinciples calculations were carried out to design and demonstrate a novel macropore graphitic carbon nitride(gC_(10)N_(3))as a promising 2D electrocatalyst substrate to support single-transition metal(TM,from Sc to Au).The"donation-acceptance"charge interaction in the TM-N_(2)moiety effectively balances the adsorption strength of oxygenated intermediates in Ni@g-C_(10)N_(3)and Rh@gC_(10)N_3,making them effective bifunctional OER/ORR electrocatalysts with IrO_(2)/Pt-beyond overpotentials being as low as 0.39/0.38 V and 0.54/0.44 V,***,they possess high stability and conductivity and are less susceptible to oxidation and corrosion under working *** guarantees high activity under ambient ***,the origin of the OER/ORR activity of TM@g-C_(10)N_(3) is explained using multilevel descriptors:intrinsic(p,Bader charge,integral crystal orbital Hamilton population(ICOHP),bond length,and d-band center(εd).In particular,for optimal Ni@g-C_(10)N_(3),the clear hybridization between the Ni-d orbital and surface O-p orbital causes the paired electrons to occupy the bonding *** enables OH~*to be adsorbed on the Ni@g-C_(10)N_(3),thereby achieving the highest catalytic performance.

关键词： First-principles calculation Oxygen evolution reaction Oxygen reduction reaction Bifunctional electrocatalysts Single-metal-atom electrocatalysts

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Catalysis by subsurface metal atoms in Al(001) through electron transfer

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National science Review 2024年第4期11卷 12-13页

作者： Bo Sun Ding Ma Beijing National Laboratory for Molecular science New Cornerstone Science Laboratory College of Chemistry and Molecular Engineering Peking University

Heterogeneous catalysis plays a crucial role in the chemical industry, which has evolved from the investigation of chemisorption to an electronic structure[1]. Diverse strategies, such as alloying,doping, and confining, have been applied to enhance the catalytic properties of active sites through electronic modulation. The electron transfer between active sites and substrates profoundly influences catalytic activity [2].

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Rational design of ZnCdS/TpPa-1-COF heterostructure photocatalyst by strengthening the interface connection in solar hydrogen production reactions

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Nano Research 2024年第3期17卷 1027-1034页

作者： Di Yang Zhi-Gang Li Xinghao Zhang Zenghuan Ren Weihan Lu Haining Liu Xiaomeng Guo Jijie Zhang Xian-He Bu Tianjin Key Laboratory of Metal and Molecule-Based Material chemistry School of Materials Science and EngineeringNankai UniversityTianjin 300350China college of chemistry and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuang 050018China State Key Laboratory of Elemento-Organic chemistry College of ChemistryNankai UniversityTianjin 300071China

ZnCdS quantum dots(QDs)are highly coveted in photocatalysis research for their exceptional visible-light responses and high light-absorption ***,their practical application is hindered by their tendency to aggregate,due to having high surface *** address this issue,herein,a heterostructure is synthesized by growing ZnCdS QDs with a size of approximately 5 nm onto the surface of a two-dimensional(2D)covalent organic framework(COF),*** approach suppresses the aggregation of the QDs and improves their *** ZnCdS/TpPa-1-COF composite exhibited a peak hydrogen evolution rate of 6244.16μmol·g^(-1)·h^(-1),which was 2.89 and 4.18 times greater than that of ZnCdS and TpPa-1-COF,*** zero-dimensional/two-dimensional(0D/2D)heterojunction formed by ZnCdS and TpPa-1-COF generates a strong interfacial force,which is attributed to the intimate contact between the *** connections accelerate charge separation,improve the utilisation of reduced electrons,and reduce the extent of agglomeration of the ZnCdS QDs,thereby resulting in high hydrogen production activity of the ***,the photocatalytic mechanism is studied using Kelvin probe force microscopy and theoretical *** study offers a novel approach for creating sulfide photocatalysts and is crucial for investigating the potential practical applications of the related photocatalysts.

关键词： covalent organic frameworks quantum dots photocatalysis hydrogen generation heterojunction

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Few-layered hexagonal boron nitride nanosheets stabilized Pt NPs for oxidation promoted adsorptive desulfurization of fuel oil

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Green Energy & environment 2024年第3期9卷 495-506页

作者： Peiwen Wu Xin Song Linlin Chen Lianwen He Yingcheng Wu Duanjian Tao Jing He Chang Deng Linjie Lu Yanhong Chao Mingqing Hua Wenshuai Zhu School of chemistry and Chemical Engineering Jiangsu UniversityZhenjiang212013China college of Chemical Engineering and environment State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum-BeijingBeijing102249China college of chemistry and Chemical Engineering Jiangxi Normal UniversityNanchang330022China college of science State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum-BeijingBeijing102249China

A few-layered hexagonal boron nitride nanosheets stabilized platinum nanoparticles(Pt/h-BNNS)is engineered for oxidation-promoted adsorptive desulfurization(OPADS)of fuel *** was found that the few-layered structure and the defective sites of h-BNNS not only are beneficial to the stabilization of Pt NPs but also favor the adsorption of aromatic *** employing Pt/h-BNNS with a Pt loading amount of 1.19 wt%as the active adsorbent and air as an oxidant,a 98.0%sulfur removal over dibenzothiophene(DBT)is achieved along with a total conversion of the DBT to the corresponding sulfones(DBTO_(2)).Detailed experiments show that the excellent desulfurization activity originates from the few-layered structure of h-BNNS and the high catalytic activity of Pt *** addition,the OPADS system with Pt/h-BNNS as the active adsorbent shows remarkable stability in desulfurization performance with the existence of different interferents such as olefin,and aromatic ***,the Pt/h-BNNS can be recycled 12 times without a significant decrease in desulfurization ***,a process flow diagram is proposed for deep desulfurization of fuel oil and recovery of high value-added products,which would promote the industrial application of such OPADS strategy.

关键词： Desulfurization Adsorption Catalytic oxidation Active adsorbent Dibenzothiophene

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Elevation response of above-ground net primary productivity for Picea crassifolia to climate change in Qilian Mountains of Northwest China based on tree rings

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Journal of Geographical sciences 2024年第1期34卷 146-164页

作者： WU Xuan JIAO Liang DU Dashi XUE Ruhong WEI Mengyuan ZHANG Peng college of Geography and environment science Northwest Normal UniversityLanzhou 730070China Key Laboratory of Resource environment and Sustainable Development of Oasis Northwest Normal UniversityLanzhou 730070China

Current ecosystem models used to simulate global terrestrial carbon balance generally suggest that terrestrial landscapes are stable and mature,but terrestrial net primary productivity(NPP)data estimated without accounting for disturbances in species composition,environment,structure,and ecological characteristics will reduce the accuracy of the global carbon ***,the steady-state assumption and neglect of elevation-related changes in forest NPP is a *** Qilian Mountains are located in continental climate zone,and vegetation is highly sensitive to climate *** quantified aboveground biomass(AGB)and aboveground net primary productivity(ANPP)sequences at three elevations using field-collected tree rings of Picea crassifolia in Qilian Mountains of Northwest *** results showed that(1)There were significant differences between AGB and ANPP at the three elevations,and the growth rate of AGB was the highest at the low elevation(55.99 t ha^(–1)10a^(–1)).(2)There are differences in the response relationship between the ANPP and climate factors at the three elevations,and drought stress is the main climate signal affecting the change of ANPP.(3)Under the future climate scenario,drought stress intensifies,and the predicted decline trend of ANPP at the three elevations from mid-century to the end of this century is–0.025 t ha^(–1)10a^(–1),respectively;–0.022 t ha^(–1)10a^(–1);At–0.246 t ha^(–1)10a^(–1),the level of forest productivity was significantly *** results reveal the elevation gradient differences in forest productivity levels and provide key information for studying the carbon sink potential of boreal forests.

关键词： global climate change tree ring aboveground net primary productivity aboveground biomass drought stress Qilian Mountains

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Fe-doped Co_(3)O_(4) nanowire strutted 3D pinewood-derived carbon: A highly selective electrocatalyst for ammonia production via nitrate reduction

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Nano Research 2024年第4期17卷 2276-2282页

作者： Xuwei Liu Chaozhen Liu Xun He Zhengwei Cai Kai Dong Jun Li Xiaoya Fan Ting Xie Xiya Yang Yonglan Luo Dongdong Zheng Shengjun Sun Sulaiman Alfaifi Feng Gong Xuping Sun Institute of Fundamental and Frontier sciences University of Electronic Science and Technology of ChinaChengdu 610054China Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education School of Energy and EnvironmentSoutheast UniversityNanjing 211189China college of chemistry Chemical Engineering and Materials ScienceShandong Normal UniversityJinan 250014China chemistry Department Frontier of ScienceKing Abdulaziz UniversityJeddah 21589Saudi Arabia

Nitrate(NO_(3)^(-)),a nitrogen-containing pollutant,is prevalent in aqueous solutions,contributing to a range of environmental and health-related *** electrocatalytic reduction of NO_(3)^(-)holds promise as a sustainable approach to both eliminating NO_(3)^(-)and generating valuable ammonia(NH_(3)).Nevertheless,the reduction reaction of NO_(3)^(-)(NO_(3)^(-)RR),involving 8-electron transfer process,is intricate,necessitating highly efficient electrocatalysts to facilitate the conversion of NO_(3)^(-)to NH_(3).In this study,Fe-doped Co_(3)O_(4) nanowire strutted three-dimensional(3D)pinewood-derived carbon(Fe-Co_(3)O_(4)/PC)is proposed as a high-efficiency NO_(3)^(-)RR electrocatalyst for NH_(3) *** within 0.1 M NaOH containing NO_(3)^(-),Fe-Co_(3)O_(4)/PC demonstrates exceptional performance,obtain an impressively large NH_(3) yield of 0.55 mmol·h^(-1)·cm^(-2) and an exceptionally high Faradaic efficiency of 96.5%at-0.5 V,superior to its Co_(3)O_(4)/PC counterpart(0.2 mmol·h^(-1)·cm^(-2),73.3%).Furthermore,the study delves into the reaction mechanism of Fe-Co_(3)O_(4) for NO_(3)^(-)RR through theoretical calculations.

关键词： Fe-doped Co_(3)O_(4) nanowire pinewood-derived carbon electrocatalytic NO_(3)-reduction NH_(3) synthesis density functional theory

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Development of a novel Eu^(3+)-doped tantalate red-emitting phosphor for w-LEDs application

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Journal of Rare Earths 2024年第8期42卷 1479-1488,I0003页

作者： Fan Zeng Jingjing Ru Bing Zhao Feiyun Guo Jianzhong Chen college of chemistry and Materials Fujian Province University Key Laboratory of Green Energy and Environment CatalysisNingde Normal University.Ningde352100China School of environment and Resources School of Carbon Neutral and Modern IndustryFujian Normal UniversityFuzhou350007China college of Information and Mechanical&Electrical Engineering Ningde Normal UniversityNingde352100China college of chemistry Fuzhou UniversityFuzhou350108China

Two novel phosphors LiBa_(4(1-x))Eu_(4x)Ta_(3)O_(12)(H-LBTO:xEu^(3+)) and Li_(0.25)Ba_(1-x)Eu_(x)Ta_(0.75)O_(3)(C-LBTO:xEu^(3+))were prepared successfully by a molten salt *** transformation between these two structures was realized by changing the sintering temperature or changing the Eu^(3+) ions concentration,which was also demonstrated by the X-ray diffraction(XRD),scanning electron microscopy(SEM),diffuse reflectance spectra(DRS),and photoluminescence excitation(PLE) analyses,Both the sintering temperature and the Eu^(3+)ions doping concentration have significant impact on the formation of the crystal *** these phosphors sintered at 1023 K exhibit two major luminescence lines at 594 and 614 nm under nearUV light of 395 nm excitation,corresponding to Eu^(3+)ions typical transitions of ^(5)D_(0)→^(7)F_(1) and ^(5)D_(0)→^(7)F_(2).The optimum concentration of Eu^(3+) ions is 9 mol% for C-LBTO:xEu^(3+) samples and the quenching interaction type is the nearest-neighbor ion *** thermal stability of the C-LBTO:0.09Eu^(3+)sample was investigated in detail and the device application further suggests that C-LBTO:0.09Eu^(3+) can be used as a red phosphor for near-UV excited w-LEDs in lighting.

关键词： Phosphor Tantalate LED device Rare earths

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Efficient and stable PtFe alloy catalyst for electrocatalytic methanol oxidation with high resistance to CO

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Journal of Energy chemistry 2024年第3期90卷 327-336,I0008页

作者： Qian Yang Sifan Zhang Fengshun Wu Lihua Zhu Guang Li Mingzhi Chen An Pei Yingliang Feng Jiangxi Provincial Key Laboratory of Functional Molecular Materials chemistry College of Chemistry and Chemical EngineeringFaculty of Materials Metallurgy and ChemistryJiangxi University of Science and TechnologyGanzhou 341000JiangxiChina college of chemistry and Chemical Engineering Xiamen UniversityXiamen 361005FujianChina

Direct methanol fuel cells(DMFC) are widely considered to be an ideal green energy conversion device but their widespread applications are limited by the high price of the Pt-based catalysts and the instability in terms of surface CO toxicity in long-term ***,the PtFe alloy nanoparticles(NPs) with small particle size(~4.12 nm) supported on carbon black catalysts with different Pt/Fe atomic ratios(Pt_(1)Fe_(2)/C,Pt_(3)Fe_(4)/C,Pt_(1)Fe_(1)/C,and Pt_(2)Fe_(1)/C) are successfully prepared for enhanced anti-CO poisoning during methanol oxidation reaction(MOR).The optimal atomic ratio of Pt/Fe for the MOR is 1:2,and the mass activity of Pt_(1)Fe_(2)/C(5.40 A mg_(Pt)^(-1)) is 13.5 times higher than that of conventional commercial Pt/C(Pt/C-JM)(0.40 A mg_(Pt)^(-1)).The introduction of Fe into the Pt lattice forms the PtFe alloy phase,and the electron density of Pt is reduced after forming the PtFe ***-situ Fourier transform infrared results indicate that the addition of oxyphilic metal Fe has reduced the adsorption of reactant molecules on Pt during the *** doping of Fe atoms helps to desorb toxic intermediates and regenerate Pt active sites,promoting the cleavage of C-O bonds with good selectivity of CO_(2)(58.1%).Moreover,the Pt_(1)Fe_(2)/C catalyst exhibits higher CO tolerance,methanol electrooxidation activity,and long-term stability than other Pt_(x)Fe_(y)/C catalysts.

关键词： Alloy catalyst PtFe Methanol oxidation In-situ FTIR CO resistance

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Towards wafer-scale growth of two-dimensional cerium dioxide single crystal with high dielectric performance

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Nano Research 2024年第9期17卷 8592-8599页

作者： Zhuofeng Shi Muhammad Imran Xiaohui Chen Xin Liu Yaqi Zhu Zhaoning Hu Saiyu Bu Jialin Zhang Chunhu Li Xiaodong Zhang Li Lin college of chemistry and Chemical Engineering Qingdao UniversityQingdao 266000China School of Materials science and Engineering Peking UniversityBeijing 100871China Center for Nanochemistry Beijing Science and Engineering Center for NanocarbonsBeijing National Laboratory for Molecular ScienceCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Key Laboratory of Marine chemistry Theory and Technology Ministry of EducationCollege of Chemistry and Chemical EngineeringOcean University of ChinaQingdao 266100China

Owing to the atomically thin nature,two-dimensional(2D)oxide materials have been widely reported to exhibit exciting transport and dielectric properties,such as fine gate controllability and ultrahigh carrier mobility,that outperform their bulk ***,unlike the successful synthesis of bulk oxide single crystals,reliable methods for synthesizing large-area single crystal of 2D oxide,that would suppress the negative influence from defective grain boundaries,remain unavailable,especially for nonlayered ***,we report that the lattice symmetry between the substrate and cerium dioxide(CeO_(2))would allow for the aligned nucleation and epitaxial growth of CeO_(2)on sapphire substrates,enabling the wafer-sized growth of CeO_(2)single *** careful tuning of the growth temperature and oxygen flow rate contributed to the harvesting of CeO_(2)wafer with reduced thickness and enhanced growth *** removal of grain boundaries improved the dielectric performance in terms of high dielectric strength(Ebd≈8.8 MV·cm^(-1)),suppressed leakage current,along with high dielectric constants(εr≈24).Our work demonstrates that with fine dielectric performance and ease of synthesizing wafer-sized single crystals,CeO_(2)can function as potential candidate as gate insulator for 2D-materials based nanoelectronics,and we believe the reported protocol of aligned nucleation can be extended to other 2D oxides.

关键词： dielectric materials two-dimensional materials chemical vapor deposition cerium dioxide

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Recovery of cyanophycin granule polypeptide from activated sludge: carbon source dependence and aggregation-induced luminescence characteristics

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Frontiers of environmental science & Engineering 2024年第2期18卷 25-34页

作者： Kui Zou Hongyuan Liu Bo Feng Taiping Qing Peng Zhang college of environment and Resources Xiangtan UniversityXiangtan 411105China

In the sewage treatment process,facilitating the conversion of pollutants into value-added resources holds great potential for reducing the amount of greenhouse gas emissions and promoting economic *** granule polypeptide(CGP),a recently discovered high value-added biopolymer present in activated sludge,has provided new avenues for the recovery of ***,the mechanisms that regulate CGP synthesis and the characteristics of this biopolymer in activated sludge remain unclear thus *** study investigated the synthesis of CGP,polyhydroxyalkanoates(PHA),and alginate-like exopolysaccharides(ALE)in various microbial aggregates under different carbon sources feeding *** results showed that the CGP yields was superior that of PHA and ALE when subjected to identical carbon source feeding ***,biofilm was more conducive to CGP accumulation than floc *** with glucose and methanol,sodium acetate significantly enriched the CGP synthetase-encoding gene(cphAabundance=~17419),resulting in the highest CGP yield(average 107.1 mg/g MLSS)in both biofilm and floc *** study is the first to reported the characteristic fluorescence of CGP(Ex/Em=~360/450 nm)caused by the aggregated luminescence of arginine on the side ***,this study highlights the potential application of CGP as a fluorescent material and offers insights into CGP recovery from activated sludge in wastewater treatment plants.

关键词： Cyanophycin Polyhydroxyalkanoate Alginate-like exopolysaccharides Bioresource recovery Aggregation-induced luminescence

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