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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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Four-birds-with-one-stone:A multifunctional Ti-based material for solar-driven water evaporation

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Nano Research 2024年第5期17卷 4498-4506页

作者： Yannan Li Yaning Sun Dan Zhang Yu Xue Jie Wang Nan Zhang Jun Wang Jiangwei Zhang Yan Zhao Jun-Jie Liu school of Physical science and Technology College of Energy Materials and ChemistryInner Mongolia UniversityHohhot 010021China

Sustainable,environmentally friendly and low-energy desalination materials have important research value for the increasing demand of freshwater year by ***,it is a huge challenge to maintain high heat energy transfer efficiency without reducing the heat conversion capacity of specific solar photothermal conversion ***,their efficiency and durability are greatly limited by the problems of seawater corrosion,oil,and bacteria *** now,no related work has been reported to solve all the aforementioned problems via a simple four-birds-with-one-stone ***,a class of multifunctional porous photothermal silver(Ag)modified Ti foams(Tf-TA/Ag series materials)is prepared for the development of advanced solar water evaporation devices,and provides alternative materials for alleviating freshwater crisis and treating *** oil contact angle(OCA)changes from 41°to 180°,which significantly reduces the adhesion of *** addition,Tf-TA2/Ag sample also shows an excellent and sustained antibacterial effect,which maintains above 99.9%of antibacterial rate after repeated 5 *** surface temperature of the Tf-TA2/Ag sample reaches 52.5℃ after simulated sun irradiation for 20 min,which is significantly higher than that of the contact groups(water:36.4℃,Ti foam:38.2℃ and Tf-TA2:40.9℃).The capacity of seawater evaporation and salt removal is enhanced due to the excellent photothermal properties,low reflectance,and uniform heat dissipation *** water production efficiency of Tf-TA2/Ag sample is 1.41 kg·m^(-2)·h^(-1) in artificial seawater and 0.76 kg·m^(-2)·h^(-1) in oily sewage under simulated sun ***,the hydrophilic and oleophobic properties of Tf-TA2/Ag are critical to extracting water from oil/water mixture in diverse water ***,this four-birds-with-one-stone approach provides a new perspective for the improvement of solar seawater desalination performance.

关键词： four-birds-with-one-stone photothermal material antibacterial material antifouling property

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Fe3O4/Fe/FeS Tri-Heterojunction Node Spawning N-Carbon Nanotube Scaffold Structure for High-Performance Sodium-Ion Battery

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Energy & Environmental Materials 2024年第4期7卷 143-152页

作者： Yuan Liu Qing Lin Xiaocui Chen Xufeng Meng Baoxiu Hou Haiyan Liu Shuaihua Zhang Ningzhao Shang Zheng Wang Chaoyue Zhang Jianjun Song Xiaoxian Zhao Department of chemistry College of Science Hebei Agricultural University college of chemistry and Chemical Engineering Qingdao University college of Physics Qingdao University

The Fe-based anode of sodium-ion batteries attracts much attention due to the abundant source,low-cost,and high specific ***,the low electron and ion transfer rate,poor structural stability,and shuttle effect of NaS2intermediate restrain its further ***,the Fe3O4/Fe/FeS tri-heterojunction node spawned N-carbon nanotube scaffold structure（FHNCS） was designed using the modified MIL-88B（Fe） as a template followed by catalytic growth and sulfidation process.

关键词： anode core-shell heterojunction hollow structure sodium ion batteries

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Additives strategies to improving cycling stability of Li metal batteries by modifying electrode electrolyte interphases

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Progress in Natural science:Materials International 2024年第2期34卷 338-344页

作者： Yuan Li Pengfei Huang Chunyu Cui Xiaoyuan Ma Li Chen Zekun Li Linhai Li Yuhong Tian school of Biological and Chemical Engineering Guangxi University of Science and Technology school of college of chemistry and Chemical Engineering Hunan University Isky Future Energy Institute

Li metal batteries（LMBs） have attracted much attention due to the ultra-high theoretical capacity of the Li metal anode（LMA）.However,the uncontrollable dendrites growth and low coulombic efficiency hinder their practical ***,we explore 3,5-difluoropyridine（2F-BD） as a novel electrolyte additive to enable highperformance *** 2F-BD additive participates in and modifies the solvation structure of Li ions by reducing the coordinated number of PF6-at the electrode surface,leading to the formation of a LiF and Li3N-rich solid electrolyte interphase（SEI）.The LiF component increases the robustness of SEI and suppresses the formation of Li dendrites,while the Li3N component facilitates the transportation and reaction kinetics of Li *** a result,the Li‖Li symmetric cell presents a stable cycling performance of up to 500 h at a current density of 1 mA *** coupling with LiFePO4cathode,the obtained full cell achieves high specific capacities of 106.06 mA h g-1and 84.98 mA h g-1at 2.55 mA cm-2and 5.10 mA cm-2,respectively,and maintains a high capacity retention of84.0% after 1000 cycles at 0.13 mA cm-2,with an average cycling CE of 99.58%.

关键词： Electrolyte additive Li dendrites Li metal batteries LiF and Li3N-Rich electrode-electrolyte interphase LiFePO4 cathode

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Two-dimensional C2N-based single-atom catalyst with complex microenvironment for enhanced electrochemical nitrogen reduction:A descriptor-based design

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Journal of Energy chemistry 2024年第10期97卷 110-119页

作者： Enduo Dai Wei An Ruixian Guo Xugen Shi Yunyi Li Yibo Wang Mingming Liu college of chemistry and Chemical Engineering Shanghai University of Engineering Science

The catalytic descriptor with operational feasibility is highly desired towards rational design of high-performance catalyst especially the electrode/electrolyte solution interface working under mild ***,we demonstrate that the descriptor Ω parameterized by readily accessible intrinsic properties of metal center and coordination is highly operational and efficient in rational design of single-atom catalyst（SAC） for driving electrochemical nitrogen reduction（NRR）.Using twodimensional metal（M）-BxPySzNm@C2N as prototype SAC models,we reveal that*N2+（H++e-）→*N2H acts predominantly as the potential-limiting step（PLS） of NRR on M-B2P2S2@C2N and M-B1P1S1N3@C2N regardless of the distinction in coordination *** the 28 screened M active sites,with Ω values close to the optimal 4,M-B2P2S2@C2N(M=V（Ω=3.53）,Mo（Ω=5.12）,and W（Ω=3.92）) and M-B1P1S1N3@C2N(M=V（Ω=3.00）,Mo（Ω=4.34）,and W（Ω=3.32）) yield the lowered limiting potential（UL） as-0.45,-0.54.-0.36,-0.58,-0.25,and-0.24 V,respectively,thus making them the promising NRR *** importantly,these SACs are located around the top of volcano-shape plot of ULversus Ω,re-validating Ω as an effective descriptor for accurately predicting the high-activity NRR SACs even with complex *** study unravels the relationship between active-site structure and NRR performance via the descriptor Ω,which can be applied to other important sustainable electrocatalytic reactions involving activation of small molecules via σ-donation and π*-backdonation mechanism.

关键词： Descriptor DFT Electrocatalysis N2 reduction Single-atom catalyst

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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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Polypyride intercalation boosting the kinetics and stability of V3O7·H2O cathodes for aqueous zinc-ion batteries

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Journal of Energy chemistry 2024年第10期97卷 361-370页

作者： Qingqing He Jie Bai Mengda Xue Yanxin Liao Huayu Wang Mujun Long Lingyun Chen Department of Applied chemistry School of Chemistry and Chemical Engineering Chongqing University Laboratory of Materials and Metallurgy College of Materials Science and Engineering Chongqing University

V3O7·H2O（VO） is a high capacity cathode material in the field of aqueous zinc ion batteries（AZIBs）,but it is limited by slow ion migration and low electrical *** this paper,polypyridine（PPyd） intercalated VO with nanoribbon structure was prepared by a simple in-situ pre-intercalation,which is noted *** total density of states（TDOS） shows that after the pre-intercalation of PPyd,an intermediate energy level appears between the valence band and conduction band,which provides a step that can effectively reduce the band gap and enhance the electron ***,the density functional theory（DFT） results found that Zn2+is more easily de-intercalated from the V-O skeleton,which proves that the embeddedness of PPyd improves the diffusion kinetics of Zn2+.Electrochemical studies have shown that VO-PPyd cathode materials exhibit excellent rate performance(high specific capacity of 465 and 192 mA h g-1at 0.2 and 10 A g-1,respectively) and long-term cycling performance（92.7%capacity retention rate after 5300 cycles）,due to their advantages in structure and *** importantly,the energy density of VO-PPyd//Zn at 581 and 5806 W kg-1is 375 and 247 W h kg-1,***-PPyd exhibits excellent electrochemical properties compared to previously reported vanadium based cathodes,which makes it highly competitive in the field of high-performance cathode materials of AZIBs.

关键词： Aqueous zinc ion batteries DFT calculation Electrical conductivity Ion migration Polypyridine V3O7·H2O

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Precise construction of RuPt dual single-atomic sites to optimize oxygen electrocatalytic behaviors for high-performance Zn-air batteries

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Journal of Energy chemistry 2024年第10期97卷 520-528页

作者： Xiaolin Hu Zhenkun Wu Chaohe Xu school of science Chongqing Key Laboratory of New Energy Storage Materials and Devices Chongqing University of Technology school of chemistry and Engineering Chongqing University college of Materials science and Engineering Chongqing University

The development of redox bifunctional electrocatalysts with high performance,low cost,and long lifetimes is essential for achieving clean energy *** study proposed an atom capture strategy for anchoring dual single atoms（DSAs） in a zinc-zeolitic imidazolate framework（Zn-ZIF）,followed by calcination under an N2atmosphere to synthesize ruthenium-platinum DSAs supported on a nitrogendoped carbon substrate（RuPt DSAs-NC）.Theoretical calculations showed that the degree of Ru 5dxz-*O 2pxorbital hybridization was high when*O was adsorbed at the Ru site,indicating enhanced covalent hybridization of metal sites and oxygen ligands,which benefited the adsorption of intermediate *** presence of the RuPtN6active center optimized the absorption-desorption behavior of intermediates,improving the electrocatalytic performance of the oxygen reduction reaction（ORR） and the oxygen evolution reaction（DER）,RuPt DSAs-NC exhibited a 0.87 V high half-wave potential and a 268 mV low overpotential at 10 mA cm-2in an alkaline ***,rechargeable zinc-air batteries（ZABs）achieved a peak power density of 171 MW *** RuPt DSAs-NC demonstrated long-term cycling for up to 500 h with superior round-trip *** study provided an effective structural design strategy to construct DSAs active sites for enhanced electrocata lytic performance.

关键词： Atom capture Dual single atoms catalysts Oxygen evolution reaction Oxygen reduction reaction Rechargeable Zn-air batteries

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Single-atom Zn confined in hierarchical hollow microstructure as an acid/base-resistant microwave absorption materials

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Nano Research 2024年第8期17卷 6785-6794页

作者： Yue Lou Jiao Li Xiaokun Li Zhenyu Zhu Zhan Shi Biao Xu school of chemistry and Chemical Engineering Nanjing University of Science and TechnologyNanjing 210094China State Key Laboratory of Inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China

Developing acid/base-resistant and low-price microwave-absorbing materials with lighter weight is highly desired for practical applications in extreme ***,we demonstrate the successful synthesis of the N-doped porous carbon(NC)material with hierarchical pore structure by the spray pyrolysis *** large specific surface area(SBET=707.53 m^(2)·g^(−1))of materials enables multiple scattering of incident electromagnetic waves,and N doping greatly enhances the electrical conductivity of the ***,single-atom Zn can adjust the local electronic structure of adjacent sites such as carbon and nitrogen atoms,induce the center of polarization,and thus change the dielectric and electronic properties of the host *** porous carbon coating of single-atom Zn avoids the deterioration of electromagnetic parameters caused by the accumulation of magnetic particles under high-temperature *** the same time,they can also be used in various complex environments,such as acidic and basic ***,NC-1000,with high surface area,low density,and good chemical stability,obtained a minimum reflection loss(RLmin)of−50.5 dB and an effective absorption bandwidth(EAB)exceeding 5.1 GHz at the thickness of 1.9 *** soaking in the strong acid and base solution,the electromagnetic wave absorption performance of the material decreased by<15%.Widely available raw materials and a simple preparation scheme are expected to expedite industrial mass production for this novel type of materials.

关键词： hierarchical hollow microstructure microwave absorption metal-organic framework(MOF) impedance matching singleatom Zn acid/base-resistant

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PVDF-assisted pyrolysis strategy for corrugated plate oxygen electrocatalysis nanoreactor:Simultaneously realizing efficient active sites and rapid mass transfer

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Journal of Energy chemistry 2024年第10期97卷 612-621页

作者： Chenxi Xu Liang Chen Haihui Zhou Shifeng Qin Zhaohui Hou Yangyang Chen Jiale Sun Junwei Xu Zhongyuan Huang college of chemistry and Chemical Engineering Hunan University college of Materials science and Technology Central South University of Forestry and Technology Key Laboratory of Hunan Province for Advanced Carbon-based Functional Materials School of Chemistry and Chemical Engineering Hunan Institute of Science and Technology

Though Zn-air batteries(ZABs) are one of the most promising system for energy storage and conversion,challenge still persists in its commercial application due to the sluggish kinetics of oxygen reduction/evolution reaction(ORR/OER).Hereby,a polyvinylidene fluoride(PVDF)-assisted pyrolysis strategy is proposed to develop a novel corrugated plate-like bifunctional electrocatalyst using two-dimensional zeolitic imidazolate frameworks(2D ZIF-67) as the *** employed PVDF plays an important role in inheriting the original 2D structure of ZIF-67 and modulating the composition of the final *** a result,a corrugated plate-like electrocatalyst,high-density Co nanoparticles decorated 2D Co,N,and F tri-doped carbon nanosheets,can be *** acquired electrocatalyst enables efficient active sites and rapid mass transfer simultaneously,thus showing appreciable electrocatalytic performance for rechargeable Zn-air ***,our proposed strategy offers a new perspective to the design of advanced oxygen electrocatalysts.

关键词： Active sites Corrugated plate Mass transfer Oxygen electrocatalyst Zn-air batteries

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