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Reduced water dissociation barrier on constructing Pt-Co/CoO_(x)interface for alkaline hydrogen evolution

Nano Research 2022年第6期15卷 4958-4964页

作者： Yandong Wang Wei Wu Runzhe Chen Caoxin Lin Shichun Mu Niancai Cheng College of Materials Science and Engineering Fuzhou UniversityFuzhou 350108China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Water dissociation process is generally regarded as the rate-limiting step for alkaline hydrogen evolution reaction(HER),and severely inhibits the catalytic efficiency of Pt based *** overcome this problem,the in-situ constructed interfaces of PtCo alloy and amorphous cobalt oxide(CoO_(x))on the carbon powder are *** amorphous CoO_(x)at Pt-Co/CoO_(x)interfaces not only provide active sites for water dissociation to facilitate Volmer step,but also produce the strong electronic transfer with ***,the obtained interfacial catalysts exhibit outstanding alkaline HER performance with a Tafel slope of 29.3 mV·dec^(−1)and an ultralow overpotential of only 28 mV at 10 mA·cm^(−2).Density functional theory(DFT)reveals that the electronic accumulation on the interfacial Co atom in Pt-Co/CoO_(x)constructing the novel active site for water *** to the Pt-Co,all of the energy barriers for water adsorption,water dissociation and hydrogen adsorption/desorption are reduced in Pt-Co/CoO_(x)interfaces,suggesting a boosted HER kinetics for alkaline HER.

关键词： interfacial construction amorphous cobalt oxide water dissociation dual active site electronic regulation

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Dynamic photoluminescence switching of carbon nitride thin films for anticounterfeiting and encryption

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Chinese Journal of Structural Chemistry 2024年第10期43卷 49-54页

作者： Hang Meng Bicheng Zhu Ruolun Sun Zixuan Liu Shaowen Cao Kan Zhang Jiaguo Yu Jingsan Xu School of Chemistry and Physics and Centre for Materials Science Queensland University of TechnologyBrisbaneQueensland4000Australia Laboratory of Solar Fuel Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan430074China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan430070China Department of Materials Science and Key Laboratory of Automobile Materials MOEState Key Laboratory of Superhard MaterialsJilin UniversityChangchun130012China

Photoluminescence(PL)has been increasingly applied in anticounterfeiting and encryption as counterfeiting becomes more ***,common luminescent encryption techniques are based on static PL mea-surements and are easy to *** this work,we have developed a thermal vapor deposition(TVD)approach using melem as the unique starting material to synthesize highly homogeneous carbon nitride(CN)thin films featuring unique dynamic PL switching *** being irradiated by a white LED,the blue PL in-tensity of the CN film increases significantly and then fades in darkness,demonstrating excellent *** results prove that CN films contain cyano groups in the structure,and density functional theory(DFT)calculations indicate that the integration of cyano groups results in traps within the bandgap of CN,sug-gesting that the dynamic PL switching effect is essentially associated with the fullness of the trap *** have therefore developed an advanced luminescent device for the secure transmission of encrypted information through controlled *** can be easily read with a portable UV(365 nm)lamp and effectively erased using the white LED,thereby preventing information leakage and showing great potential for many applications.

关键词： Thermal vapor deposition Carbon nitride film Dynamic photoluminescence Encryption

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Effects of a novel refiner Al-3Ti-4.35La combined with Sr on microstructure and mechanical properties of as-cast A356 alloy

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China Foundry 2024年第6期21卷 641-650页

作者： Mei Xu Wan-wu Ding Li-wen Hu Shi-hao Chen Hai-xia Zhang Hai-cun Yu Wen-jun Zhao School of Materials Science and Engineering Lanzhou University of TechnologyLanzhou 730050China State Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals Lanzhou University of TechnologyLanzhou 730050China

It is a practically significant issue to refine and modify industrial Al-Si casting alloy to improve its *** the present study,a novel refiner Al-3Ti-4.35La alloy,prepared by a melt-reaction method,was used,combined with Sr to refine the as-cast A356 *** effects on the as-cast microstructures and mechanical properties of A356 alloy were *** results indicate that the combined addition of Al-3Ti-4.35La intermediate alloy and Sr can improve the microstructure and enhance the mechanical properties of A356 *** adding 0.3wt.%Al-3Ti-4.35La and 0.03wt.%Sr to the as-cast A356 alloy,the average grain size ofα-Al decreases from 693.47μm to 264.13μm(a decrease of 61.91%),the secondary dendrite arm spacing(SDAS)is decreased by 47.8%from 32.09μm to 16.75μm,and the eutectic Si is transformed from an acicular structure to short rods and a granular *** ultimate tensile strength(UTS)and elongation(EL)of the as-cast A356 alloy modified by Al-3Ti-4.35La and Sr reach 216.3 MPa and 10.6%,which are enhanced by 29.54%and 134.66%compared with the unmodified alloy,*** fracture mode is transformed from transgranular fracture to intergranular fracture,and the ductile toughness of the alloy is *** adding the Al-3Ti-4.35La and Sr,the undercooling for the nucleation ofα-Al and eutectic Si increases,leading to an accelerated nucleation rate and an increased number of nuclei,which shortens the duration of the eutectic reaction and consequently inhibits grain growth.

关键词： A356 alloy Al-3Ti-4.35La Sr refiner grain refinement microstructure mechanical properties

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Single-atom Cu anchored on N-doped graphene/carbon nitride heterojunction for enhanced photocatalytic H_(2)O_(2) production

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Journal of materials Science & technology 2023年第30期161卷 192-200页

作者： Han Li Bicheng Zhu Bei Cheng Guoqiang Luo Jingsan Xu Shaowen Cao State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Laboratory of Solar Fuel Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430078China School of Chemistry and Physics Queensland University of TechnologyBrisbaneQLD 4000Australia

Photocatalytic production of H_(2)O_(2) by polymeric carbon nitride has been regarded as a promising ap-proach for the conversion of solar energy into valuable ***,the efficiency of pristine car-bon nitride is limited by the rapid charge recombination and the lack of suitable active ***,we introduce single-atom Cu anchored on N-doped graphene(Cu-NG)as a cocatalyst coupled with carbon nitride via covalent bonding to enhance photocatalytic H_(2)O_(2) *** Cu-NG/carbon nitride could broaden the light absorption from UV to near-infrared region,contributing to the photocatalytic ***,NG containing electron-rich N atoms could serve as anchoring sites for stabilizing single-atom ***,the single-atom Cu acts not only as an electron sink to steer the interfacial charge sep-aration but also as an active site for molecular oxygen adsorption and *** the synergistic effect of the enhanced interfacial charge separation and suitable active sites,Cu-NG/carbon nitride ex-hibits improved photocatalytic performance with an H_(2)O_(2) generation rate of 2856μmol g^(−1)h^(−1),which is 2.6 times that of pristine carbon *** work provides a protocol for high-performance photocat-alytic H_(2)O_(2) production using a single-atom cocatalyst.

关键词： Single-atom catalysis Interfacial charge separation Photocatalytic H_(2)O_(2)production

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Micro-strain regulation strategy to stabilize perovskite lattice based on the categories and impact of strain on perovskite solar cells

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Journal of Energy Chemistry 2025年第1期100卷 578-604页

作者： Caixia Li Wenwu Liu Shiji Da Lingbin Kong Fen Ran State Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals Lanzhou University of TechnologyLanzhou 730050GansuChina School of Materials Science and Engineering Lanzhou University of TechnologyLanzhou 730050GansuChina

Photovoltaic metal halide perovskite solar cells(PSCs) convert light to electricity more efficiently than crystalline silicon cells, and the cost of materials used to make them is lower than that of silicon *** efficiency is not a core issue affecting the application of perovskite solar cells in special *** present, stability is the major technical encounters that hinders its further commercial development. Microstrain in PSCs is currently a significant factor responsible for the device's instability. Strain-induced ion migration is widely believed to accelerate perovskite degradation even when external stimuli are ***, it is imperative to study strain to enhance the stability of PSCs. This paper reviews recent developments to understand strain's origin and effect mechanisms on performance of PSCs, including ion migration,failure behavior, defect formation, and its effect on photoelectric properties, stability, and ***, several well-known strain management strategies are systematically introduced based on the strain effect mechanism and strain engineering on the film, providing more clues for further preparation with increased stability. The manipulation of external physical strain applied from films to entire devices has been extensively studied. Furthermore, recommendations for future research directions and chemical approaches have been provided. It is emphasized that strain engineering plays a crucial role in improving the efficiency and longevity of PSCs. Tensile strain causes rapid degradation, while moderate compressive strain and external strain control could improve properties and stability. Efforts should focus on controlling compressive strain to mitigate residual tensile strain and introducing it in a controlled manner. Future research endeavors may focus on exploring these pathways to improve the efficiency and lifespan of PSCs.

关键词： Halide perovskite solar cells Strain origins Strain effects Strain management

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Defect chemistry and thermal conductivity of the εSmO_(1.5)·(1−ε)ZrO_(2)(0.2≤ε≤0.65)ceramics:Effect of the nonstoichiometry

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Journal of advanced Ceramics 2024年第11期13卷 1823-1834页

作者： Zhixue Qu Tong Zhang Wei Pan Key Laboratory of Advanced Functional Materials Education Ministry of ChinaCollege of Materials Science and EngineeringBeijing University of TechnologyBeijing 100124China State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and EngineeringTsinghua UniversityBeijing 100084China

Rare-earth zirconate pyrochlores,which exhibit various interesting properties,especially low thermal conductivity,are of great *** is an effective strategy involving defect engineering to reduce the thermal conductivity of *** this work,a long series of solid solutions,εSmO_(1.5)·(1−ε)ZrO_(2)(ε=0.200,0.250,0.350,0.400,0.450,0.500,0.525,0.550,0.600,and 0.650),were designed and synthesized to investigate the effects of nonstoichiometry on the structural evolution,defect chemistry,and thermal conductivity of SmO_(1.5)–ZrO_(2) system across the entire pyrochlore phase field and phase transition *** similarity of all the Raman spectra provides an incredible opportunity to confirm the structural details and evolution of pyrochlore and defective fluorite,as well as the emergence of the expected point defects.A new solution mechanism concerning nonstoichiometry was proposed and confirmed by analyzing the variations in the experimental density and Raman *** thermal conductivities of all the samples were measured,and investigated in terms of the phonon-scattering *** results show that the nonstoichiometry with SmO1.5 excess is more effective in reducing the thermal conductivity to an extremely low value of approximately 1 W/(m·K),which can be attributed to the dramatic decrease in the average acoustic velocity in addition to the strong phonon scattering of Zr ion vacancies and oxygen *** the other hand,the nonstoichiometry with ZrO_(2) excess significantly reduces the thermal conductivity at room temperature,but conversely leads to a slight increase of it above 200°*** former variation can be attributed to the phonon scattering of the 8a interstitial oxygen ions,which has a similar effectiveness to the defects on the SmO1.5-rich *** latter variation may be attributed to the Umklapp scattering of phonons.

关键词： nonstoichiometry pyrochlore rare-earth zirconate thermal conductivity defect chemistry

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Multiscale Anion-Hybrid in Atomic Ni Sites for High-Rate Water Electrolysis: Insights into the Charge Accumulation Mechanism

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Journal of the American Chemical Society 2024年第20期146卷 14194-14202页

作者： Li, Yan Peng, Yanan Dong, Wenda Jiang, Xueyu Lu, Lijun Yang, Dali Hsu, Liang-Ching Li, Wu Su, Baolian Lei, Aiwen Wuhan University Hubei Wuhan430072 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Hubei Wuhan430070 China National Chung Hsing University Taichung40227 Taiwan

Single-atom catalysts, characterized by transition metal-(N/O)4 units on nanocarbon (M-(N/O)4-C), have emerged as efficient performers in water electrolysis. However, there are few guiding principles for accurately controlling the ligand fields of single atoms to further stimulate the catalyst activities. Herein, using the Ni-(N/O)4-C unit as a model, we develop a further modification of the P anion on the outer shells to modulate the morphology of the ligand. The catalyst thus prepared possesses high activity and excellent long-term durability, surpassing commercial Pt/C, RuO2, and currently reported single-atom catalysts. Notably, mechanistic studies demonstrated that the pseudocapacitive feature of multiscale anion-hybrid nanocarbon is considerable at accumulating enough positive charge [Q], contributing to the high oxygen evolution reaction (OER) order (β) through the rate formula. DFT calculations also indicate that the catalytic activity is decided by the suitable barrier energy of the intermediates due to charge accumulation. This work reveals the activity origin of single atoms on multihybrid nanocarbon, providing a clear experiential formula for designing the electronic configuration of single-atom catalysts to boost electrocatalytic performance. © 2024 American Chemical Society.

关键词： Catalyst activity

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A flame-retardant binder with high polysulfide affinity for safe and stable lithium–sulfur batteries

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Science China Chemistry 2024年第3期67卷 1028-1036页

作者： Guowei Yu Guofeng Ye Cheng Wang Chenyang Wang Zhaoyun Wang Pu Hu Yu Li Xi-Xi Feng Shuang-Jie Tan Min Yan Sen Xin Zhitian Liu Hubei Key Laboratory of Plasma Chemistry and Advanced Materials Hubei Engineering Technology Research Center of Optoelectronic and New Energy MaterialsSchool of Materials Science and EngineeringWuhan Institute of TechnologyWuhan 430205China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China CAS Key Laboratory of Molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular SciencesBeijing National Laboratory for Molecular Sciences(BNLMS)Institute of ChemistryChinese Academy of Sciences(CAS)Beijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Lithium-sulfur(Li-S) batteries have shown promises for the next-generation, high-energy electrochemical storage, yet are hindered by rapid performance decay due to the polysulfide shuttle in the cathode and safety concerns about potential thermal runaway. To address the above challenges, herein, we show a flame-retardant cathode binder that simultaneously improves the electrochemical stability and safety of batteries. The combination of soft and hard segments in the polymer framework of binders allows high flexibility and mechanical strength for adapting to the drastic volume change during the Li(de)intercalation of the S cathode. The binder contains a large number of polar groups, which show the high affinity to polysulfides so that they help to anchor active S species at the cathode. These polar groups also help to regulate and facilitate the Li-ion transport, promoting the kinetics of polysulfide conversion reaction. The binder contains abundant phosphine oxide groups, which, in the case of battery's thermal runaway, decompose and release PO· radicals to quench the combustion reactions and stop the fire. Consequently, Li-S batteries using the new cathode binder show the improved electrochemical performance, including a low-capacity decay of 0.046% per cycle for 800 cycles at 1 C and favorable rate capabilities of up to 3 C. This work offers new insights on the practical realization of high-energy rechargeable batteries with stable storage electrochemistry and high safety.

关键词： lithium–sulfur battery polymer binder polysulfide affinity flame retardancy

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Serrated lithium fluoride nanofibers-woven interlayer enables uniform lithium deposition for lithium-metal batteries

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National Science Review 2022年第11期9卷 194-207页

作者： Shuangshuang Tan Yalong Jiang Shuyan Ni Hao Wang Fangyu Xiong Lianmeng Cui Xuelei Pan Chen Tang Yaoguang Rong Qinyou An Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology College of Materials Science and Engineering Chongqing University Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory

The uncontrollable formation of Li dendrites has become the biggest obstacle to the practical application of Li-metal anodes in high-energy rechargeable Li batteries. Herein, a unique LiF interlayer woven by millimeter-level, single-crystal and serrated LiF nanofibers（NFs） was designed to enable dendrite-free and highly efficient Li-metal deposition. This high-conductivity Li F interlayer can increase the Li+transference number and induce the formation of 'Li F–NFs-rich' solid–electrolyte interface（SEI）. In the 'Li F–NFs-rich'SEI, the ultra-long Li F nanofibers provide a continuously interfacial Li+transport path. Moreover, the formed Li–LiF interface between Li-metal and SEI film renders low Li nucleation and high Li+migration energy barriers, leading to uniform Li plating and stripping processes. As a result, steady charge–discharge in a Li//Li symmetrical cell for 1600 h under 4 m Ah cm-2and 400 stable cycles under a high area capacity of 5.65 mAh cm-2in a high-loading Li//rGO–S cell at 17.9 mA cm-2could be achieved. The free-standing LiF –NFs interlayer exhibits superior advantages for commercial Li batteries and displays significant potential for expanding the applications in solid Li batteries.

关键词： lithium fluoride serrated nanofibers LiF interlayer uniform Li deposition lithium-metal batteries

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Reduced graphene oxide-induced in-situ uniform growth of hydrated WO_(3) film for enhanced electrochromic performance

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Nano Research 2025年第4期18卷 569-577页

作者： Rui Fang Yang Liu Chunyu Shi Huihui Jin Zibo Chen Haohao Sun Ben Lv Daping He Xusheng Zheng Yuli Xiong State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and EngineeringWuhan University of TechnologyWuhan 430070China School of Science Wuhan University of TechnologyWuhan 430070China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China Sanya Science and Education Innovation Park of Wuhan University of Technology Sanya 572000China School of Materials Science and Engineering Wuhan University of TechnologyWuhan 430070China

WO_(3)-graphene electrochromic materials are widely used in electrochromic devices including smart windows and electronic displays,due to their ability to adjust optical transmittance in the visible and near-infrared ranges under low electrode ***,the uniformity of the film remains a challenge for the widely used physical mixing-coating *** this study,we present a two-dimensional material-assisted synthesis of a porous hydrated WO_(3) film(WH-rGO)based on reduced graphene oxide(rGO)nanosheets and WO_(3)(rGO-WO_(3))seed layer via a hydrothermal *** incorporation of rGO not only promotes the uniform growth of hydrated WO_(3) film,enhancing ion transport but also introduces oxygen vacancies,creating an efficient conduction pathway for charge *** resulting WH-rGO film exhibits impressive performance,achieving 71% optical modulation at 700 nm,with bleaching and coloring times of 4.2 and 1.0 *** coloration efficiency is calculated at 156.11 cm^(2)·C^(-1),and the optical modulation is maintained at 93% of the initial optical modulation after 1000 cycles applied in the +1.0 and -1.1 V potential *** work offers new insights into the role of oxygen vacancies in enhancing the electrochromic properties of hydrated WO_(3) films through the addition of *** also provides a promising approach for the synthesis of electrochromic materials,facilitating their application in smart window technologies.

关键词： electrochromic film hydrated tungsten oxide reduced graphene oxide oxygen vacancy

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