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Trace of Atomically Dispersed Pd Enables Unprecedented Butadiene Semihydrogenation Performance Over Copper Catalyst

ACS Catalysis 2025年第5期15卷 3810-3822页

作者： Zhao Wang Hao Yuan Jian Tao Shu-Lin Liu Ying Hong Zhi-Yi Hu Jian Zhang Bao-Lian Su The State Key Laboratory of Advanced Technology for Material Synthesis and Processing Wuhan University of Technology Wuhan Hubei 430070 P. R. China State Key Laboratory of Solidification Processing School of Materials Science and Engineering Northwestern Polytechnical University Xi’an Shaanxi 710000 P. R. China The State Key Laboratory of Advanced Technology for Material Synthesis and Processing Wuhan University of Technology Wuhan Hubei 430070 P. R. China；Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles Namur B-5000 Belgium

Semihydrogenation plays a key role in industrial hydrorefining of light alkenes, with a market above 400 billion by 2027. The high cost of commercial palladium-based catalysts strongly calls for innovation but with great challenges. Herein, copper nanoparticles decorated with a minimized ppm of Pd are developed through a chemical plating process to integrate the catalytic advantages of copper and palladium for achieving maximized catalysis in the semihydrogenation of a fatal impurity of butadiene in alkene feedstocks. The developed Pd–Cu catalyst (i.e., 114 ppm of Pd in Pd0.0033Cu1/TiO2) exhibits an unprecedented catalytic performance superior to commercial Pd/Al2O3, with 100% butene selectivity above 90% of butadiene conversion over 130 h on stream at 90 °C. Further exploration reveals that the atomically dispersed Pd on Cu nanoparticles, obtained at ultralow ppm levels of Pd loading, induces a hidden but critical H2trap, which concentrates H2on the Pd site for further H2dissociation that offers intermediate hydrogen atoms to the tandem butadiene semihydrogenation over the third layer of Cu atoms neighboring Pd through hydrogen spillover. Moreover, a threshold on Pd density was identified at Pd/Cu surficial atomic ratio of 1/138 (i.e., Pd0.0033Cu1/TiO2) for maximizing butadiene semihydrogenation performance, based on an extreme collaboration between Pd for H2dissociation and Cu for butadiene hydrogenation. This work provides important guidance for developing noble metal-saving catalysts in industrial applications.

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Ionic liquid engineering enabled in-plane orientated 1D perovskite nanorods for efficient mixed-dimensional perovskite photovoltaics

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InfoMat 2023年第8期5卷 81-93页

作者： Fei Wang Dawei Duan Kang Zhou YZBXue Xiao Liang Xianfang Zhou Chuangye Ge Chao Zhou Jin Xiang Jiajie Zhu Quanyao Zhu Haoran Lin Yumeng Shi Yonghua Chen Gang Li Hanlin Hu Hoffmann Institute of Advanced Materials Shenzhen PolytechnicShenzhenthe People's Republic of China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and EngineeringWuhan University of TechnologyWuhanthe People's Republic of China Oxford Instruments Technology(Shanghai)Co.Ltd. Shanghaithe People's Republic of China International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education Institute of Microscale OptoelectronicsShenzhen UniversityShenzhenthe People's Republic of China School of Physics Science and Engineering Tongji UniversityShanghaithe People's Republic of China Key Laboratory of Flexible Electronics(KLoFE)&Institute of Advanced Materials(IAM) School of Flexible Electronics(Future Technologies)Nanjing Tech University(NanjingTech)Nanjingthe People's Republic of China Department of Electronic and Information Engineering Research Institute for Smart Energy(RISE)The Hong Kong Polytechnic UniversityKowloonHong Kongthe People's Republic of China

Mixed-dimensional engineering of perovskite material has been demonstrated as a facile and promising strategy to improve both photovoltaic performance and long-term stability of perovskite solar cells(PSCs).In this study,we report an in-plane preferred orientation of 1D perovskite induced by an ionic liquid(IL)of 1-(3-cyanopropyl)-3-methylimidazolium chloride(CPMIMCl)for the first time via sequential deposition approach,leading to a mixed dimensional perovskite thin *** generated one-dimensional(1D)CPMIMPbI3 with in-plane orientation resides at the grain boundaries of three-dimensional(3D)perovskite can be appreciably observed from the morphology level,leading to creation of high-quality films with large grain size with more efficient defect ***,the dispersion of IL in the bulk phase of perovskite material allows for the formation of 1D perovskite for multiple level passivation to inhibit non-radiative recombination and optimize carrier *** IL engineering strategy not only yields a mixed-dimensional perovskite heterostructure with in-plane orientation 1D perovskite nano-rods but also significantly improves the opto-electronic property with suppressed trap *** a result,the CPMIMCl-treated PSCs show an enhanced photovoltaic performance with a champion power conversion efficiency(PCE)up to 24.13%.More importantly,benefiting from the hydrophobicity of formed 1D perovskite and defects suppression,the corresponding PSC demonstrates an excellent longterm stability and maintain 97.1%of its pristine PCE at 25C under 50%RH condition over 1000 *** research provides an innovative perspective for employing the low dimensional engineering to optimize the performance and stability of photovoltaic devices.

关键词： 1D/3D perovskite ionic liquid perovskite solar cells stability

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Additive Engineering in Spray Enables Efficient Methylammonium-Free Wide-Bandgap Perovskite Solar Cells

SSRN

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SSRN 2023年

作者： Chen, Xiao Geng, Cong Yu, Xinxin Feng, Yishuai Liang, Cheng Peng, Yong Cheng, Yibing State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Hubei Wuhan430070 China

Spray coating is an emerging technique, paving the way for the commercialization of perovskite. However, it still faces challenges in the preparation of wide-bandgap (WBG) perovskite solar cells (PSCs) for tandem photovoltaic devices. Applying a two-step evaporate-spray method, and an additive engineering strategy, where n-propylammonium chloride is introduced in spray processing, we fabricate efficient and stable methylammonium-free (MA-free) WBG PSCs. The propylammonium cation plays a role in passivating grain boundaries, which resulted in the reduction of vacancy defects on the surface of films. Cl- plays a big part in the crystal growth process. After the addition of PACl, preferred crystalline orientation, larger grain size, and reduced trap density in perovskite films are obtained. Finally, the champion WBG PSC (Energy gap (Eg), Eg≈1.68 eV) delivers a power conversion efficiency (PCE) over 19%, which is the highest efficiency of the WBG PSCs prepared by the evaporate-spray method, as compared to pristine devices with the highest PCE of 16.59%. Additionally, the barrier against moisture formed at the surface of films significantly enhances humidity stability of the photovoltaic (PV) device. © 2023, The Authors. All rights reserved.

关键词： Additives

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Three dimensional porous frameworks for lithium dendrite suppression

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Journal of Energy Chemistry 2020年第5期29卷 73-89页

作者： Shuyan Ni Shuangshuang Tan Qinyou An Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina

Lithium metal is a promising anode material owing to its very low electrochemical potential and ultrahigh specific ***,the growth of lithium dendrites could result in a short lifespan,low coulombic efficiency,and potential safety hazards during the progress of lithium plating/*** factors drastically hinder its application in lithium metal *** review focuses on the use of three dimensional(3D)porous host frameworks to improve Li plating/stripping behaviors,accommodate the change in volume,and suppress or block lithium dendrite *** 3D porous frameworks,including the conductive carbon-based,metal-based,and lithiophilic inorganic-compound frameworks are introduced and summarized in *** particular functions,relative developments,and optimized strategies of various 3D porous frameworks for lithium deposition/dissolution behaviors are ***,the challenges and promising developments in the field of Li metal anodes will be discussed at the end of this review.

关键词： Lithium metal battery 3D porous frameworks Lithium dendrite Lithium sulfur batteries Lithium oxygen batteries Li plating/stripping

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Operating conditions combination analysis method of optimal water management state for PEM fuel cell

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Green Energy and Intelligent Transportation 2023年第4期2卷 28-42页

作者： Wenxin Wan Yang Yang Yang Li Changjun Xie Jie Song Zhanfeng Deng Jinting Tan Ruiming Zhang School of Automation Wuhan University of TechnologyWuhan430070China Hubei Key Laboratory of Advanced Technology for Automotive Components Wuhan University of TechnologyWuhan430070China Department of Electrical Engineering Chalmers University of TechnologyGothenburg41258Sweden Modern Industry College of Artificial Intelligence and New Energy Vehicles Wuhan University of TechnologyWuhan430070China Global Energy Interconnection Research Institute Beijing102211China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan430070China Guangdong Hydrogen Energy Institute of Wuhan University of Technology Foshan528000China

The water content of proton exchange membrane fuel cells(PEMFCs)affects the transport of reactants and the conductivity of the *** water management measures can improve the performance and extend the lifespan of the fuel *** water management state of the stack is influenced by various external operating conditions,and optimizing the combination of these conditions can improve the water management state within the *** that the stack's internal resistance can reflect its water management state,this study first establishes an internal resistance-operating condition model that considers the coupling effect of temperature and humidity to determine the variation trend of total resistance and stack humidity with single-factor operating ***,the water management state optimization method based on the ANN-HGPSO algorithm is proposed,which not only quantitatively evaluates the influence weights of different operating conditions on the stack's internal resistance but also efficiently and accurately obtains the optimal combination of five operating conditions:working temperature,anode gas pressure,cathode gas pressure,anode gas humidity,and cathode gas humidity to achieve the optimal water management state in the stack,within the entire range of current ***,the response surface experimental results of the stack also validate the effectiveness and accuracy of the ANN-HGPSO *** method mentioned in this article can provide effective strategies for efficient water management and output performance optimization control of PEMFC stacks.

关键词： PEMFC Water management statue Internal resistance-operating condition model Operating condition optimization Response surface method

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Boosting the electrochemical performance and reliability of conducting polyme microelectrode via intermediate graphene for on-chip asymmetric micro-supercapacitor

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Journal of Energy Chemistry 2020年第10期29卷 224-232页

作者： Muhammad Tahir Liang He Wei Yang Xufeng Hong Waqas Ali Haider Hui Tang Zhe Zhu Kwadwo Asare Owusu Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina

High-performance anode is hurdle for on-chip planar microsupercapacitor(MSC).Polypyrrole(PPy)is a highly attractive pseudocapacitive material,but its low cycling stability,and low adhesion with current collector hinder its *** we propose one-prong generic strategy to boost the cycling stability of *** our strategy,the electrochemical deposition of multilayered reduced graphene oxide(rGO)on micropatterned Au is utilized,and the resultant rGO@Au pattern is then used for growing highly porous PPy nanostructures by facile electrochemical *** fabricated PPy anode on rGO@Au has quasi rectangular cyclic voltammetry curves up to-0.7 V and exceptional cycling stability,retaining82%of capacitance after 10,000 charge/discharge cycles in 2 M KCl *** outstanding reliability of PPy on rGO@Au is due to the flexibility of rGO,accommodating structural pulverization and providing a promising background for the nucleation of highly porous ***,an all-polymer based asymmetric aqueous MSC(AMSC)is constructed with PPy anode and PEDOT cathode,which exhibited excellent electrochemical performance compared with conventional symmetric MSCs based on conducting *** constructed AMSC delivered a maximum areal capacitance of 15.9 m F cm^-2(99.3 F cm^-3),high specific energy and power densities of 4.3μWh cm^-2(27.03 mWh cm^-3)and 0.36 W cm^-2(0.68 W cm^-3)at 1.4 V,*** enhanced electrochemical performances can be illustrated by nucleation mechanism,in which surface topology of r GO generates a promising background for nucleation and electrochemical growth of nanoporous pseudocapacitive conducting polymers with superior interfacial contact and improved surface area.

关键词： Electrochemical polymerization Nucleation Asymmetric microsupercapacitors

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Two-dimensional gersiloxenes with tunable band gap as new photocatalysts

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Rare Metals 2020年第6期39卷 610-612页

作者： Shao-Wen Cao State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Designing highly efficient and stable photocatalysts is of vital importance for solar-to-fuel conversion,as a potential strategy to address the concerns of global energy crisis and environmental *** development of novel photocatalytic materials is desirable to overcome those shortcomings of traditional semiconductor photocatalysts.

关键词： catalysts overcome shortcomings

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Awakening the oxygen evolution activity of MoS_(2) by oxophilic-metal induced surface reorganization engineering

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Journal of Energy Chemistry 2021年第11期30卷 546-551,I0013页

作者： Xueqin Mu Yang Zhu Xiangyao Gu Shipeng Dai Qixin Mao Lintao Bao Wenxuan Li Suli Liu Jianchun Bao Shichun Mu Jiangsu Key Laboratory of Biofunctional Materials School of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023JiangsuChina Key Laboratory of Advanced Functional Materials of Nanjing Nanjing Xiaozhuang UniversityNanjing 211171JiangsuChina State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu hydrogen ValleyFoshan 528200GuangdongChina

Although molybdenum disulfide (MoS_(2))-based materials are generally known as active electrocatalysts for the hydrogen evolution reaction (HER), the inert performance for the oxygen evolution reaction (OER) seriously limits their wide applications in alkaline electrolyzers due to there exists too strong metal-sulfur (M−S) bond in MoS_(2). Herein, by means of surface reorganization engineering of bimetal Al, Co-doped MoS_(2) (devoted as AlCo_(3)-MoS_(2)) through in situ substituting partial oxidation, we successfully significantly activate the OER activity of MoS_(2), which affords a considerably low overpotential of 323 mV at −30 mA cm^(−2), far lower than those of MoS_(2), Al-MoS_(2) and Co-MoS_(2) catalysts. Essentially, the AlCo_(3)-MoS_(2) substrate produces lots of M−O (M=Al, Co and Mo) species with oxygen vacancies, which trigger the surface self-reconstruction of pre-catalysts and simultaneously boost the electrocatalytic OER activity. Moreover, benefiting from the moderate M−O species formed on the surface, the redistribution of surface electron states is induced, thus optimizing the adsorption of OH* and OOH* intermediates on metal oxyhydroxides and awakening the OER activity of MoS_(2).

关键词： Surface reorganization engineering Porous nanosheets Oxygen evolution reaction MoS_(2) Oxophilic-metal

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Microstructure and tribological properties of -oriented 3C-SiC by chemical vapor deposition

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Ceramics International 2025年

作者： Yang, Wenxuan Huang, Wei Li, Cuicui Wang, Chongjie Zhang, Chitengfei Tu, Rong Zhang, Song Hubei Longzhong Laboratory No.101 Luming Road Xiangyang441000 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China Hubei Technology Innovation Center for Advanced Composites Wuhan430070 China

Highly -oriented 3C-SiC coatings were fabricated by chemical vapor deposition method at different temperatures. As deposition temperature increased from 1473 K to 1773 K, the surface structure of -oriented 3C-SiC transitioned from hexagonal structure with sixfold symmetry to hill-like structure, and finally to conical porous surface composed of stacked short rods. Owing to alteration of surface structure, the hardness of 3C-SiC coatings presented a trend of initially increasing and subsequently decreasing. The 3C-SiC coating deposited at 1673 K possessed the highest hardness, with a value of 42.08 GPa. The average friction coefficient for 3C-SiC/Si3N4 pair ranged from 0.258 to 0.569. The wear rate and hardness exhibited opposite trends. Compared with 3C-SiC coatings prepared at the other three temperatures, the 3C-SiC coating deposited at 1573 K exhibited the lowest wear rate under loads of 5 N, 10 N, and 15 N. Furthermore, the lowest wear rate, recorded at 15 N, was 4.1 × 10−6 mm3/Nm, attributed to high hardness and uniform grain size. The wear mechanism of -oriented 3C-SiC coatings during dry sliding primarily involved fracture, leading to fatigue and third-body wear. © 2025 Elsevier Ltd and Techna Group S.r.l.

关键词： Rockwell hardness

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Molecular origin for toughness of hydrogel artificial spider silk for surgical sutures

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Science China Chemistry 2025年

作者： Jiatian Li Abdul Qadeer Khan Weiqiang Zhao Zhipeng Lai Qiankun Bao Muhammad Rafique Fazhi Ye Jie Bai Qiang Zhou Liqiang Mai Zongqian Wang Enzhao Liu Xiang Zhou Zunfeng Liu Chemical Engineering College Inner Mongolia University of Technology Tianjin Key Laboratory of Ionic-Molecular Function of Cardiovascular Disease Department of Cardiology Tianjin Institute of CardiologyThe Second Hospital of Tianjin Medical University State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer Materials Tianjin Key Laboratory of Functional Polymer Materials College of Chemistry Nankai University School of Biomedical Engineering and Med-X Research Institute Shanghai Jiao Tong University State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Tianjin First Central Hospital School of Textile and Garment Anhui Polytechnic University Department of Science School of Traditional Chinese Pharmacy China Pharmaceutical University

The pursuit of biomimetic fibers with simultaneous high toughness and strength persists, despite their inherent ***, for artificial spider silk based on gel fiber, it is still unclear for the molecular chain attributes related to the improvement of the strength and toughness. Here, a hydrogel fiber was prepared by mimicking the molecular structure of natural spider silk, and we delved into the molecular chain structure characteristics related to the strength, toughness and damping capacity of gel fiber, such as crosslinking density, molecular chain orientation and hydrogen bond interaction. The results indicate that a certain increase in crosslinking density and molecular chain orientation contributes to the enhancement of tensile strength, while the toughness and damping remain essentially unaltered. The thermal dissociation of hydrogen bond could enhance the toughness in a specific range, while the humidity destruction of hydrogen bond would reduce the *** well-regulation control of the weight ratio of polyacrylamide （PAM） to poly（acrylic acid）(PAA), the PAM@PAA gel fibers could reach maximum breaking strength of 1.02 GPa, maximum toughness of 149 MJ m-3, and damping capacity of 95%.PAM@PAA gel fiber has demonstrated excellent wound healing performance and biocompatibility in vivo evaluation as a surgical suture, which indicates its potential in biomedical applications.

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