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Boosting the Antioxidant Efficiency of Ce(Iii)-Based Organometallic Complexes Via Ion-Limited Domain and Electronic Structure Modulation Towards Robust Proton Exchange Membrane Fuel Cells

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SSRN 2023年

作者： Zhao, Shengqiu Liao, Yucong Wang, Rui Li, Hao Zhang, Haining Tang, Haolin State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China Foshan Xianhu Laboratory The Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen Valley Foshan528200 China

Ce-based radical scavengers, including free Ce3+, are highly efficient radical scavengers with rapid and regenerative redox properties that can enhance the chemical durability of prton exchange membranes (PEMs). However, during the proton exchange membrane fuel cell (PEMFC) operation, water-soluble free Ce3+ ions in PEMs irreversibly migrate away and poison the proton-conducting ion clusters, leading to a decline in PEMFC output power. Herein, organometallic complexes of Ce3+ ions (Ce/HMCRE) derived by Ce3+ ions coordinating with 2-hydroxymethyl-15-crown-5 ether (HMCRE) ligands were utilized as FRS for improving the stability of PEMs. Owing to the coordination between the crown ether oxygen atom of the ligand and the Ce3+, the migration of Ce3+ and the adverse interactions among Ce3+ ions with the sulfonic group of PEM was inhibited. Meanwhile, the formation of coordination bonds allows the central Ce3+ ion to accept electrons on the ligand oxygen atom, thus enhancing the antioxidant efficiency of Ce/HMCRE. Gratifyingly, the hydrogen bonding between the hydroxymethyl group of the HMCRE ligand and the ether oxygen atom on the side chain of the perfluorosulfonic acid (PFSA) matrix also contributes to anchoring the Ce/HMCRE complex and mitigating its interference with ion clusters of PEM. Consequently, the Ce/HMCRE-based hybrid PEMs demonstrated an OCV decay rate of 0.45 mV h-1, a maximum power density of 1.07 W cm-2, an H2 crossover value of 2.41 mA cm-2, a thickness retention of 92% after 150 hours of accelerated degradation testing. © 2023, The Authors. All rights reserved.

关键词： Ligands

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Manipulating micro-electric field and coordination-saturated site configuration boosted activity and safety of frustrated single-atom Cu/O Lewis pair for acetylene hydrochlorination

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Nano Research 2023年第7期16卷 9039-9049页

作者： Junchen Peng Dandan Dong Zongyuan Wang Hong Yang Dongyang Qiao Qinqin Wang Wei Sun Minmin Liu Jiajun Wang Mingyuan Zhu Bin Dai Fei He Chaofeng Huang School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering Shihezi UniversityShihezi 832000China School of Chemistry and Chemical Engineering Southeast UniversityNanjing 211189China School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin UniversityTianjin 300072China College of Chemistry&Chemical Engineering Yantai UniversityYantai 264010China School of Material Science and Engineering University of JinanJinan 250022China

Simultaneously boosting acetylene hydrochlorination activity and avoiding formation of explosive copper acetylide over Cu-based catalyst,which represented a promising alternative to Hg-based and noble metal catalysts,remained ***,we fabricated a frustrated single-atom Cu/O Lewis pair catalyst(Cu/O-FLP)by coupling epoxide group(C-O-C)with atomdispersed Cu-cis-N_(2)C_(2)Cl center to address this *** basic epoxy site modulated the electron-deficient state of Lewisacidic Cu center and paired with the Cu-cis-N_(2)C_(2)Cl moiety to preferentially break HCl into different electronegative Cu-Clδ-and C-O-H^(δ+)intermediates,which further induced both an extra localized electric field to polarize acetylene and a upshift of the dband center of catalyst,thereby promoting adsorption and enrichment of acetylene by enhancing the dipolar interaction between acetylene and active ***,the generated Cu-Clδ-and C-O-H^(δ+)drastically reduced the energy barrier of ratelimiting step and made vinyl chloride easier to desorb from the Lewis-basic oxygen-atom site rather than traditional Lewis-acidic Cu *** superiorities ensured a higher activity of Cu/O-FLP compared with its ***,preferential dissociation of HCl endowed single-atom Cu with the coordination-saturated configuration,which impeded formation of explosive copper acetylide by avoiding the direct interaction between Cu and acetylene,ensuring the intrinsic safety during catalysis.

关键词： acetylene hydrochlorination Lewis pair single-atom Cu site configuration electric field

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Refined platelet size: Unlocking enhanced mechanics in nacre-mimetic mineralized materials

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Nano Today 2025年 62卷

作者： Chen, Wei Ma, Yuanyuan Xu, Shiqing Wang, Yang Zhang, Pengchao Meng, Jingxin Fu, Zhengyi Wang, Shutao CAS Key Laboratory of Bio-inspired Materials and Interfacial Science Technical Institute of Physics and Chemistry Chinese Academy of Sciences Beijing100190 China Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and Engineering Wuhan University of Technology Wuhan430070 China University of Chinese Academy of Sciences Beijing100049 China

Nacre-mimetic mineralized (NMM) materials with outstanding mechanical properties have been considered as future structural materials. However, replicating nacre's characteristics into artificial ones in mild conditions has been challenging, particularly in controlling the platelet size, which is crucial for mechanical performance. Here, inspired by mollusk biomineralization, we achieve the unprecedented regulation of aragonite platelet sizes (ranging from 76 to 5800 μm2) at the micrometer scale by manipulating amorphous nano calcium carbonate content, thereby enhancing the mechanical properties of NMM materials. Experimental and simulation results demonstrate that merely decreasing the aragonite platelets' sizes can significantly increase the flexural strength and modulus by 2.8 and 9.9 times, respectively. Notably, the proposed strategy not only has the potential for large-scale production but also produces refined NMM material that closely resembles natural nacre in terms of microstructure and mechanical properties, showing ca. 26 % improvement in specific strength over previously reported NMM materials. Consequently, this work provides a feasible way for developing advanced biomimetic structural materials with specific functions, such as protective gear and artificial bone grafts. © 2025 Elsevier Ltd

关键词： Biomimetic mineralization Mechanical property Nacre-mimetic materials Platelet size

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Confined Tuning of the Charge Distribution of Pt Electrocatalyst for Reinforcing Anti-Poisoning Ability: Toward Efficient Separation of Hydrogen from Gases Containing Ammonia

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SSRN 2023年

作者： Jin, Changqing Wu, Fanglin Tang, Haibo Pan, Hongfei Chen, Zhida Wang, Rui Meng, Zihan Li, Junsheng Tang, Haolin State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China Foshan Xianhu Laboratory of the Advanced Energy Science Technology Guangdong Laboratory Xianhu Hydrogen Valley Foshan528200 China

The development of catalysts for hydrogen oxidation reaction (HOR) with enhanced resistance to ammonia poisoning is an important factor in the practical application of hydrogen electrochemical purification devices (HEPDs). This paper reports on the creation of a highly active and anti-ammonia HOR catalyst developed by tuning the charge distribution of the support material through nitrogen-doping of carbon. The nitrogen-doped carbon-supported platinum catalyst (Pt-N2/KB, 2.03 wt.% Pt) achieves a high mass activity and exchange current density of 2788 mA mgpt-1 and 1020 mA mgpt-1, respectively, which are 5.4 and 4.7 times higher than that of the comm. 20% Pt/C. The Pt-N2/KB catalyst also displays a lower percentage of current decay and enhanced electrochemical stability, indicating superior anti-ammonia toxicity in the tests with HEPD. Density functional theory (DFT) calculations reveal that the hydrogen adsorption free energy (ΔGH*) on the surface of Pt-N2/KB is close to zero and has a lower ammonia adsorption energy, thus accounting for its superior HOR activity and anti- ammonia poisoning ability. Consequently, this work facilitates the implementation of HOR catalysts for anti-ammonia poisoning in the HEPDs, thus accelerating the advancement of ammonia cracking for hydrogen production. © 2023, The Authors. All rights reserved.

关键词： Ammonia

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Microwave synthesis and enhancement of thermoelectric performance in Hf_(x)Ti_(1-x)NiSn_(0.97)Sb_(0.03)half-Heusler bulks

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Rare Metals 2023年第11期42卷 3780-3786页

作者： Ying Lei Yu Li Run-Dong Wan Wen Chen Hong-Wei Zhou School of Metallurgical Engineering Anhui University of TechnologyMaxiang RoadMa’anshan243032China College of Materials Science and Engineering Kunming University of Science and TechnologyKunming650093China Institute of Mineral Resources Development and Utilization Changsha Research Institute of Mining and Metallurgy Co.LtdChangsha410012China State Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals Lanzhou University of TechnologyLanzhou730050China Department of Mechanical Engineering Blekinge Institute of Technology37179KarlskronaSweden

We obtained TiNiSn-based half-Heusler Hf_(x)Ti_(1-x)NiSn_(0.97)Sb_(0.03)bulks with 85%-96%relative densities via 5-min microwave synthesis and 20-min microwave sintering in sealed *** phase composition and microstructure of samples were characterized by X-ray diffractometer(XRD)and scanning electron microscopy(SEM).Thermoelectric(TE)properties were measured,i.e.,Seebeck coefficient(S),electrical resistivity(ρ),and thermal conductivity(κ)through Seebeck coefficient/resistance analysis system(S/RAs)and laser flash thermal analyzer(LFT).The results show that the nearly single phase exists after microwave *** grain sizes and the number of grain boundaries decrease with increase in Hf-doping amount due to an increase in point *** matrix grains for Hf_(0.1)Ti_(0.9)NiSn_(0.97)Sb_(0.03)are~10μ*** nanoscle pores and precipitates are present as second phases in matrix *** real composition for Hf_(0.1)Ti_(0.9)NiSn_(0.97)Sb_(0.03)matrix grain is Hf_(3.51)Ti_(28.76)-Ni_(34.76)Sn_(31.55)Sb_(1.43).The variation trends of electrical resistivity,Seebeck coefficient,power factor,and thermal conductivity were analyzed in *** maximum figure of merit(ZT)of 0.46 is obtained for Hf_(0.1)Ti_(0.9-)NiSnSn_(0.97)Sb_(0.03)at 723 *** innovation route exhibits advantages for predation of TE bulks when compared to the conventional methods,especially in terms of efficiency while it still maintains TE performance.

关键词： Half-Heusler alloys Microwave synthesis Hf doping Thermoelectric figure of merit

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Construction of an Anti-Anionic-Depletion Layer to Mitigate the Tip Deposition Effect for Dendrite-Free Zinc Anode

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SSRN 2024年

作者： Li, Xiaohui Qiu, Dan Zhou, Qiancheng Yang, Ze Zhou, Xing Wang, Wenping Wei, Chenchen Zou, Ting Yu, Ying Institute of Nanoscience and Nanotechnology College of Physical Science and Technology Central China Normal University Wuhan430079 China State Key Laboratory of Advanced Technology for Materials Synthesis and processing Wuhan University of Technology Wuhan430070 China

Rechargeable aqueous zinc-ion batteries have been plagued by the well-known problem of zinc dendrite formation. This issue mainly arises from the inherent depletion of anions in the vicinity of the zinc anode during deposition process, leading to a strong spatial electric field that influences Zn2+ cations deposition and triggers dendrite growth. Herein, the anti-anionic-depletion strategy is proposed that involves anions anchored in the surface region of zinc anode to mitigate the adverse effects of the spatial electric field and inhibit dendrite growth. By theoretical calculations and experimental verification, layered double hydroxides (LDHs) materials were selected to immobilize SO42- anions and construct a protective coating layer against anion depletion (anti-anionic-depletion layer). Furthermore, the deposition flux of Zn2+ cations was also regulated by in-situ growing LDH nanosheets. Benefiting from these modifications, the in-situ grown ZnAl-LDH modified electrode (Zn@ZnAl) exhibits outstanding stability (5500 cycles at 40 mA cm-2), and shows negligible capacity degradation in both Zn-Mn full cells and zinc hybrid capacitors. © 2024, The Authors. All rights reserved.

关键词： Positive ions

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Tribological properties of plasma-sprayed nickel alloy matrix self-lubricating coating at elevated temperatures

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Rare Metals 2021年第7期40卷 1844-1850页

作者： Wen-Sheng Li Yang Sun Wei Hu Sheng-Yu Zhu Hai-Min Zhai Jun Yang Xiang-Juan Fan Wei-Min Liu State Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals School of Materials Science and EngineeringLanzhou University of TechnologyLanzhou 730050China State Key Laboratory of Solid Lubrication Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China

A nickel alloy matrix high-temperature self-lubricating coating(77.5 wt%(Ni-Cr-Mo-Al)-12.5 wt%Ag-10 wt%BaF2/CaF2)was prepared by plasma spraying *** show that the Vickers microhardness of coating is(2.9±0.5)GPa,and the average bonding strength is about(35.6±0.5)*** coating rubbing against Inconel 718 superalloy pin exhibits superior tribological performance with coefficient of friction(COF)of below 0.25 and wear rate of 8.2×10^(-5)-15.2×10^(-5)mm^(3)·N^(-1)·m^(-1)at a wide temperature range from 25 to 800℃,and the COF and the wear rate are slightly reduced with temperature *** low COF and wear rate were attributed to the synergistic effects of Ag,BaF_(2)/CaF_(2),Ag2MoO_(4)and BaMoO_(4).

关键词： Coating Tribological behavior High temperature Self-lubricating

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Intrinsic ion migration-induced susceptible two-dimensional phase-transition memristor with ultralow power consumption

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Science Bulletin 2025年

作者： Qin, Lanhao Yu, Yimeng Fang, Cheng Liu, Yujie Zhu, Kaichen Ouyang, Decai Liu, Shenghong Song, Bailing Zhou, Ruochen Lanza, Mario Hu, Wenhua Wu, Jinsong Li, Yuan Zhai, Tianyou State Key Laboratory of Materials Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan430074 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China Center of Hydrogen Science State Key Laboratory of Metal Matrix Composites School of Materials Science and Engineering Innovation Center for Future Materials Shanghai Jiao Tong University Shanghai200240 China Physical Science and Engineering Division King Abdullah University of Science and Technology Thuwal23955-6900 Saudi Arabia School of Computer Science and Artificial Intelligence Wuhan University of Technology Wuhan430070 China

Two-dimensional (2D) phase-transition memristors have demonstrated transformative potential for neuromorphic computing, yet challenges like high power consumption, limited endurance, and crystal damage from external ion intercalation persist. Here, we introduce a novel 2D phase-transition memristor leveraging a paradigm-shifting mechanism by exploiting the ultrafast intrinsic Cu+ ion migration within Cu2S. This approach eliminates the need for external ion insertion, significantly reducing crystal damage and enabling exceptional cycling stability with over 400 DC cycles and 500 pulse cycles. The susceptible monoclinic-tetragonal phase-transition induced by intrinsic Cu+ migration achieves an unprecedented SET power consumption of 1 μW at 100 mV, significantly lower in currently reported phase-transition memristors. To further demonstrate the potential of intrinsic ion migration-induced (IIM) memristor, we simulated an IIM memristor crossbar array for image preprocessing in gesture recognition with a high SSIM value of 0.94, showcasing its potential for scalable neuromorphic hardware. This work establishes a new paradigm in low-power, high-performance phase-transition memristors, advancing their practical application in next-generation computing. © 2025 Science China Press

关键词： Memristor Neuromorphic device Two-dimensional materials

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Screen and discovery of 10-component high-entropy borides composed of IV-VI group transition metals and rare earth elements

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Journal of materials Science & technology 2026年 242卷 226-237页

作者： Zifan Zou Liang Xu Ji Zou Shuaihang Qiu Jingjing Liu Wei Ji Wenwen Wu Zhenhao Han Weimin Wang Zhengyi Fu State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China Hubei Longzhong Laboratory Wuhan University of Technology Xiangyang Demonstration Zone Xiangyang 441000 China School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 China School of Physics and Information Technology Shaanxi Normal University Xi’an 710062 China

High-entropy borides (HEBs) are emerging as promising candidates for extreme environmental applications due to their exceptional thermal stability, mechanical properties, and tunable electromagnetic properties. This study presents the first systematic investigation of rare-earth-doped deca-component high-entropy borides, (TM 0.9 RE 0.1 )B 2 , (TM = Zr, Hf, Nb, Ta, Ti, W, Cr, V, Mo and RE = Sc, Y, Gd, Dy, Ho, Er, Lu, Sm, Eu, Tm, Tb, Pr, Yb). Evaluations of multiple descriptors, including electron work function and mixing enthalpy, revealed that Sc-containing decaboride (HEB10-Sc) exhibits superior single-phase formation capability. In contrast, the widely used valence electron concentration parameter proved inapplicable due to identical outer-electron counts across rare-earth elements. Boro/carbothermal reduction (BCTR) experiments at 1650 °C, employing transition metal oxides, rare-earth oxides, and B 4 C as precursors, demonstrated that Sc uniquely enables the formation of a single-phase diboride with nine Group IVB-VIB transition metals, unlike other rare-earth dopants. The phase evolution mechanism during the BCTR process was elucidated: ScBO 3 , formed in situ during BCTR, exhibits greater reducibility resistance than the most refractory HfO 2 , thereby suppressing polyboride formation (common in other rare-earth systems) and facilitating single-phase HEB10 formation. The resulting HEB10-Sc displays outstanding electromagnetic wave absorption performance, achieving a reflection loss (RL) of −35.3 dB at 10.6 GHz (3 mm thickness) and an effective absorption bandwidth of 4.7 GHz in the X and Ku bands. These findings underscore the critical role of rare-earth doping in tailoring the structural and functional properties of high-entropy borides, offering a pathway to design advanced multifunctional materials for extreme environments such as thermal protection and high-temperature electromagnetic absorption in aerospace and electronic applications.

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Cu(OAc)_(2)-Mediated synthesis of Fullerodihydropyridine-3-ones via the Reaction ofFullerene with β-Substituted Ethylamines in the Absence or Presence of Arylacetaldehydes

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Chinese Journal of Chemistry 2023年第13期41卷 1557-1565页

作者： Xiu-Shan Liu Hui-Juan Wang Fei-Lun Wu Jing-Wen Huo Xing-Yu Wang Fa-Bao Li Rui Sun Li Liu Chao-Yang Liu State Key Laboratory of Biocatalysis and Enzyme Engineering School of Life SciencesHubei UniversityWuhanHubei430062 China State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics Wuhan Center for Magnetic ResonanceWuhan Institute of Physics and MathematicsInnovation Academy for Precision Measurement Science and TechnologyChinese Academy of SciencesWuhanHubei430071 China Collaborative Innovation Center for Advanced Organic Chemical Materials Co-constructed by the Province and Ministry Ministry of Education Key Laboratory for the Synthesis and Application of Organic Functional MoleculesCollege of Chemistry and Chemical EngineeringHubei UniversityWuhanHubei430062 China

A series of unreported fullerodihydropyridine-3-ones were synthesized as a new family of fullerene derivatives in moderate to good yields by a simple one-step reaction of[60]fullerene with cheap and readily available β-substituted ethylamines in the absence or presence of arylacetaldehydes under the assistance of Cu(OAc)_(2).The in situ generation of arylacetaldehydes by the C—N bond cleavage of arylethylamines avoided their complex synthesis in advance and realized the preparation of fullerodihydropyridine-3-ones with structural and functional diversities,which may have promising applications in perovskite solar cells to improve the performance of photovoltaic devices due to the existence of a largeπ-conjugated system on the dihydropyridine-3-one ring.

关键词： Fullerenes Copper β-Substituted ethylamines Arylacetaldehydes Fullerodihyd ropyridine-3-ones Radical reactions

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