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Complementary enhancement between noble metal-like Fe 3 C and Cu 0 /Cu + sites to fulfil highly selective wide-potential nitrate electroreduction to ammonia

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Journal of Energy Chemistry 2025年 108卷 713-723页

作者： Yuxuan Zhou Runlin Xia Ran Hao Shengjing Li Xinyu Chen Yuping Liu Wei Li State Key Laboratory of Element-Organic Chemistry Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) College of Chemistry Nankai University Tianjin 300071 China Institute of Chemical Industry of Forest Products Chinese Academy of Forestry National Engineering Research Center of Low-Carbon Processing and Utilization of Forest Biomass Key Lab. of Chemical Engineering of Forest Products National Forestry and Grassland Administration Nanjing 210042 Jiangsu China

Mild electrocatalytic nitrate reduction reaction (NO3RR), driven by renewable electricity, is regarded as a desirable strategy for green ammonia synthesis and simultaneous removal of nitrogen-containing environmental pollutants. In view of different supply voltages from renewable energy sources, developing cost-effective and efficient electrocatalysts with a wide operating potential window is very meaningful for practical application. However, currently reported catalysts usually need to introduce noble metals to synergistically achieve wide-potential selective ammonia synthesis from nitrate. In this work, we present for the first time a dual-transition-metal electrocatalyst (Fe 3 C-CuO x @NC, x = 0, 1) with wide-potential-adaptability for highly selective nitrate reduction to ammonia. Such Fe 3 C-CuO x @NC with spatially separated CuO x and noble-metal-like Fe 3 C nanoparticles encapsulated with nitrogen-doped graphitized carbon, exhibits outstanding performance in NO3RR with desirable NH 3 Faraday efficiency of more than 90% over a wide potential ranging from −0.2 V vs. RHE to −0.6 V vs. RHE, comparable to the reported noble metal catalysts. Different from common tandem catalysis, the wide-potential high ammonia selectivity of Fe 3 C-CuO x @NC is dominantly ascribed to the complementary enhancement between CuO x and Fe 3 C, fully supported by results of experiments and density function theory calculations. CuO x exhibit highly intrinsic nitrate reduction to nitrite to compensate for the slow potential determination step (*NO 3 → *NO 3 H) of Fe 3 C, while Fe 3 C, besides behaving like noble metals to supply adequate active hydrogens, has both good adsorption and reduction abilities for nitrite species to ammonia. Moreover, Fe 3 C partially stabilizes active Cu 0 /Cu + sites, and the unique carbon-layer encapsulation structure effectively prevents the agglomeration and corrosion of metal nanoparticles during the electrocatalysis, thus maintaining good cyclic stabi

关键词： Electrolytic reduction

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ZnxCd1–xS quantum dot with enhanced photocatalytic H2-production performance

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Chinese Journal of Catalysis 2021年第1期42卷 15-24页

作者： Rongrong Gao Bei Cheng Jiajie Fan Jiaguo Yu Wingkei Ho State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001HenanChina Department of Science and Environmental Studies The Education University of Hong KongHong KongChina

H2 is an important energy carrier for replacing fossil fuel in the future due to its high energy density and environmental *** a sustainable H2-generation method,photocatalytic H2 production by water splitting has attracted much ***,oil-soluble ZnxCd1-xS quantum dot(ZCS QD)with a uniform particle size distribution were prepared by a hot-injection ***,no photocatalytic H2-production activity was observed for the oil-soluble ZCS QD due to its ***,the oil-soluble ZCS QD was converted into a water-soluble ZCS QD by a ligand-exchange *** water-soluble ZCS QD exhibited excellent photocatalytic H2-production performance in the presence of glycerin and Ni^2+,with an apparent quantum efficiency of 15.9%under irradiation of 420 nm ***,the photocatalytic H2-generation activity of the ZCS QD was~10.7 times higher than that of the ZnxCd1-xS relative samples prepared by the conventional co-precipitation *** work will inspire the design and fabrication of other semiconductor QD photocatalysts because QD exhibits excellent separation efficiency for photogenerated electron-hole pairs due to its small crystallite size.

关键词： ZnxCd1-xS Solid-solution photocatalyst Photocatalytic H2 production Oil-soluble quantum dot Water-oil soluble quantum dot

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Activating lattice oxygen of two-dimensional MnXn-1O2 MXenes via zero-dimensional graphene quantum dots for water oxidation

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Science China materials 2022年第11期65卷 3053-3061页

作者： Yiyuan Ma Yurong An Zhuo Xu Laifei Cheng Wenyu Yuan Science and Technology on Thermostructural Composite Materials Laboratory School of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072China State Key Laboratory of Solidification Processing School of Material Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072China Shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy TechnologyInstitute for Advanced Energy MaterialsSchool of Materials Science and EngineeringShaanxi Normal UniversityXi’an 710119China Key Laboratory of Macromolecular Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid ChemistrySchool of Chemistry&Chemical EngineeringShaanxi Normal UniversityXi’an 710062China

The poor oxygen evolution reaction(OER)activity of two-dimensional(2 D)transition metal carbides(MXenes)is a major obstacle to their application in highperformance water splitting and fuel cells due to the high energy barriers for the absorption of ***,we demonstrate that the lattice oxygen of M_(n)X_(n-1)O_(2)MXenes can be activated by 0 D graphene quantum dots(GQDs),thereby activating the OER via the lattice-oxygen oxidation mechanism(LOM)instead of the conventional adsorbate evolving *** pH-dependent OER activity of M_(n)X_(n-1)O_(2)@GQDs and ^(18)O isotope-lab.lling experiments with time-of-flight secondary-ion mass spectrometry(TOF-SIMS)provide the direct evidence of ***,the activated lattice oxygen amount can be controlled by the *** as-prepared 0 D/2 D Ti_(3)C_(2)O_(2)@GQDs heterostructure delivers a highly reduced overpotential of 390 mV(bare Ti_(3)C_(2)O_(2):530 mV)at a benchmark current density of 10 mA cm^(-2).Through optimizing the thickness and the additional conductive substrate,the overpotential at 10 mA cm^(-2)decreases to 250 mV,while the Tafel slope is reduced to 39 mV dec^(-1);these values indicate the as-prepared heterostructure is superior to the state-of-the-art MXene-based OER *** work provides a new strategy to enhance the OER activity of M_(n)X_(n-1)O_(2)and extends the application of LOM from perovskite to MXenes.

关键词： graphene quantum dots lattice-oxygen activation oxygen evolution reaction water splitting heterostructure

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Peridynamic stress is the static first Piola-Kirchhoff Virial stress

arXiv

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arXiv 2022年

作者： Li, Jun Li, Shaofan Lai, Xin Liu, Lisheng State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China Department of Civil and Environmental Engineering University of California BerkeleyCA94720 United States Hubei Key Laboratory of Theory and Application of Advanced Materials Mechanics Wuhan University of Technology Wuhan430070 China

The peridynamic stress formula proposed by Lehoucq and Silling [1, 2] is cumbersome to be implemented in numerical computations. Here, we show that the peridynamic stress tensor has the exact mathematical expression as that of the first Piola-Kirchhoff static Virial stress originated from Irving-Kirkwood-Noll formalism [3, 4] through the Hardy-Murdoch procedure [5, 6], which offers a simple and clear expression for numerical calculations of peridynamic stress. Several numerical verifications have been carried out to validate the accuracy of proposed peridynamic stress formula in predicting the stress states in the vicinity of the crack tip and other sources of stress concentration. The peridynamic stress is evaluated within the bond-based peridynamics with prototype microelastic brittle (PMB) material model. It is found that the PMB material model may exhibit nonlinear constitutive behaviors at large deformations. The stress fields calculated through the proposed peridynamic stress formula show good agreements with finite element analysis results, analytical solutions, and experimental data, demonstrating the promising potential of derived peridynamic stress formula in simulating the stress states of problems with discontinuities, especially in the bond-based peridynamics. Copyright © 2022, The Authors. All rights reserved.

关键词： Continuum mechanics

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Cu–N–C support confinement stabilizes active Co sites in oxygen reduction reaction

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Nano Research 2025年第5期18卷 134-144页

作者： Zhang, Longyang Sang, Wei Wang, Tingting Mu, Shichun Wei, Xiaoyu Li, Zihan Chen, Cheng Kou, Zongkui State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China Sanya Science and Education Innovation Park of Wuhan University of Technology Sanya572000 China School of Mathematical and Physical Sciences Wuhan Textile University Wuhan430200 China

Strengthening the operational durability of oxygen reduction reaction (ORR) catalysts is essential for advancing both fuel cells and metal–air batteries. However, developing highly active and durable catalysts remains a significant challenge. In this study, a catalyst (Co/Cu–N–C) featuring uniformly distributed Co nanoparticles (NPs) and Co/Cu sites has been synthesized via a facile complexassisted pyrolysis strategy. We observed that Cu–N–C support effectively confines the growth and leaching of Co NPs during both synthesis and ORR catalysis, thereby boosting the stability of the catalyst. Meanwhile, the presence of Co NPs and Cu sites slightly contributes to the ORR activity by optimizing the *OH desorption. The assembled zinc–air battery (ZAB) demonstrates a superhigh power density of 256.1 mW·cm−2 and a long-term operational stability exceeding 500 h. This work not only underscores the potential of bimetallic systems and NPs in enhancing catalyst stability but also provides valuable insights for the synthesis of high-performance ORR electrocatalysts. © The Author(s) 2025.

关键词： Electrolytic reduction

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Multifunctional Subnanowires Modulating In Situ Polymerization for High-Voltage Solid-state Batteries

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ACS applied materials & interfaces 2025年第23期17卷 2025 May 29页

作者： Haoran Xu Hong Zhang Wei Peng Shijie Feng Chenhui Dong Zixin Xiao Wei Yang Ahmed Eissa Abdelmaoula Salah Abdelghany Eleissawy Salman Chunhua Han Lin Xu State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 China. Mining and Metallurgical Department Faculty of Engineering Al-Azhar University Naser City 11884 Cairo Egypt. Hubei Longzhong Laboratory Wuhan University of Technology (Xiangyang Demonstration Zone) Xiangyang 441000 Hubei China. Hainan Institute Wuhan University of Technology Sanya 572000 China. Zhongyu Feima New Material Technology Innovation Center (Zhengzhou) Co. Ltd. Zhengzhou 450001 China.

polymerized poly(1,3-dioxolane) (PDOL) electrolytes endow excellent interfacial contact and satisfactory compatibility in lithium metal batteries (LMBs). However, their limited oxidative stability hinders compatibility with high-voltage cathodes. Herein, an effective molecular weight modulation-induced strategy via multifunctional subnanowires (SNWs) was proposed to realize the superior oxidative stability of PDOL electrolytes with narrow molecular weight distribution (MWD). Specifically, the ring-opening polymerization of DOL was promoted by oxygen vacancies (Ov) on SNWs, which enhanced the monomer conversion rate. Simultaneously, the polymerization speed during the process was regulated by the weak adsorption of monomers induced by protonated oleylamine (PO). Furthermore, the dual Lewis acid sites (Ov and PO) of the SNWs facilitate lithium salt dissociation, releasing more movable Li for transport. Thus, the SNWs-induced polymerized PDOL electrolytes with an MWD of 1.42 exhibit remarkable oxidative stability exceeding 5.1 V while achieving a lithium-ion transference number of 0.81. Consequently, the assembled NCM811||Li cells maintain a stable operation for 100 cycles at 4.5 V with a capacity retention rate of 89.2%. This research first modulates the MWD of polymerized PDOL electrolytes using subnanowires to enhance their oxidative ability, presenting a unique strategy to inspire the development of high-performance LMBs.

关键词： high-voltage in situ ring-opening polymerization molecular weight modulation solid-state lithium batteries subnanowires

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Proportion Dependent Osteogenic Activity of Electrospun Nano-Hydroxyapatite/Polylactic Acid Fiber Membrane in Vitro and in Vivo

SSRN

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SSRN 2022年

作者： Liang, Bangbang Feng, Tianyi Yuan, Xiaoting Zhao, Kang Li, Chengyu Han, Yingchao State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Biomedical Materials and Engineering Research Center of Hubei Province Wuhan University of Technology Wuhan430070 China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen Valley Foshan528200 China

Herein, nano-hydroxyapatite(nHAP) of 0-20wt% was incorporated in polylactic acid(PLA) to construct nHAP/PLA electrospun fiber membrane, and the effects of nHAP on the physicochemical properties and osteogenic activities were investigated, aiming to optimize the proportion of nHAP/PLA for a better bone repair effect. Results showed that nHAP was approximately evenly incorporated in PLA fiber and increased the fiber surface hydrophilicity. The composite membrane displayed a nHAP content-dependent mechanical property with the maximum enhancements of 29.1%, 113.2% and 45.8% in tensile strength, breaking elongation and Young’s modulus, respectively. Biological experiments demonstrated the nHAP content-dependent osteogenic activity of nHAP/PLA fiber membrane. The nHAP of 6-10wt% in membrane presented a significant promotion effect on the proliferation and differentiation of BMSCs. In vivo experiments of stacked implantation of membrane displayed the multilayer growth in pure PLA group due to the hydrophobicity of PLA resulting interlayer space and single-layer growth in nHAP/PLA group because of the hydrophilicity improved adhesion of layers. However, the 6-10wt%nHAP/PLA could promote cell recruitment and infiltration, and increase the osteogenesis with enhancements of 41% in BV/TV and 37% in BMD, respectively. Our study provides helpful supports for the preparation of composite electrospun membrane with improved osteogenic activity by optimizing the organic-inorganic proportion. © 2022, The Authors. All rights reserved.

关键词： Nanocomposites

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Regulating electron transfer through imine linkage orientations in two-dimensional covalent organic frameworks for efficient electrochromism

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Chemical Engineering Journal 2025年 516卷

作者： Wenping Shi Jing Zhou Yuli Xiong Wen Chen State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 PR China

Two-dimensional covalent organic frameworks (2D-COFs) based on imine linkages have been shown to offer intriguing optical and electrochromic (EC) performance, attracting extensive attention in the field of advanced photo-electrochemistry. However, few studies have explored how the orientation of imine linkages in 2D-COFs regulates electron transfer behavior and subsequently affects EC performance. In this work, we report an isomeric pair (Py-C-TP-COF and Py-N-TP-COF), differing only in the orientations of the imine linkages. Experimental and theoretical results demonstrate that significant differences in the electronic orbital contributions and bandgaps of 2D-COFs with distinct imine linkage orientations. Furthermore, the different orientations of imine linkages play a crucial role in the distribution of the highest occupied and the lowest unoccupied molecular orbital (HOMO and LUMO), thus significantly influencing electron separation and charge transfer. This approach of altering imine linkage orientations allows for the fine control of the charge transport and band structure of the 2D-COFs. As a result, the Py-C-TP-COF film exhibits excellent EC performance with high coloration efficiency (η CE ,1316 cm 2 ·C -1 ), fast switching time (2.0/0.4 s) and outstanding cycling stability (99.5 % retention of EC cyclic stability after 150 cycles). This study provides new insights for further rational design and optimization of functional COFs as EC materials with atomically regulated charge transfer.

关键词： Charge effective separation Covalent organic frameworks Electrochromism Electron transfer Imine linkage orientation

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Machine-Learning Modeling of Elemental Ferroelectric Bismuth Monolayer

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Physical Review Letters 2024年第26期133卷 266103-266103页

作者： Yanxing Zhang Xinjian Ouyang Dangqi Fang Shaojie Hu Laijun Liu Dawei Wang School of Physics Henan Normal University Xinxiang 453007 China School of Microelectronics & State Key Laboratory for Mechanical Behavior of Materials Xi’an Jiaotong University Xi’an 710049 China Key Lab of Micro-Nano Electronics and System Integration of Xi’an City Xi’an Jiaotong University Xi’an 710049 China MOE Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed Matter School of Physics Xi’an Jiaotong University Xi’an 710049 China Department of Physics Kyushu University 744 Motooka Fukuoka 812-8581 Japan Key Laboratory of Nonferrous Materials and New Processing Technology Ministry of Education College of Materials Science and Engineering Guilin University of Technology Guilin 541004 China

The bismuth monolayer has recently been experimentally identified as a novel platform for the investigation of two-dimensional single-element ferroelectric system. Here, we model the potential energy surface of a bismuth monolayer by employing a message-passing neural network and achieve an error smaller than 1.2 meV per atom. Empowered by the high accuracy and fast prediction of the machine learning model, we have embarked on in-depth and large-scale atomistic simulations. These explorations are tailored to understand the temperature-dependent phase transitions, with an emphasis on the difference between free-standing monolayers and those constrained by a substrate. Furthermore, with the large system used in the simulations, we are also able to observe ferroelectric domains within these systems and shed light on their intrinsic lattice thermal conductivity.

关键词： Ferroelectricity

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Solid-state Stepwise Temperature-Programmable synthesis of Bioinspired Fe-N-C Oxygen Reduction Electrocatalyst Featuring Fe-N5 Configuration

SSRN

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SSRN 2024年

作者： Sang, Wei Chaemchuen, Somboon Zhang, Longyang Wang, Zechen Li, Xingchuan Nagasaka, Cocoro Andrew Xiong, Mo Ogiwara, Naoki Chen, Cheng Verpoort, Francis Mu, Shichun Kou, Zongkui State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road Wuhan430070 China Department of Basic Science School of Arts and Sciences The University of Tokyo Komaba Meguro-ku Tokyo153-8902 Japan MOE Key Laboratory for Non-Equilibrium Synthesis and Modulation of Condensed Matter School of Physics Xi’an Jiao tong University Xi’an710049 China Sanya Science and Education Innovation Park of Wuhan University of Technology Sanya572000 China

The bioinspired Fe-N-C features an asymmetric Fe-N5 configuration to produce active metal-oxygen intermediates by introducing axial N ligand into a symmetric Fe-N4 structure, enabling highly active oxygen reduction reaction (ORR). However, the artificial creation of active Fe-N5 configuration with a direct, facile and green method is still pendent, as current techniques involve complex processes and costly precursors. Herein, we develop a novel solid-state stepwise temperature-programmable (SST) route to directly produce bioinspired Fe-N5-C. We then demonstrate that Fe-N5-C exhibit a quite higher half-wave potential (0.92 V) with 22-fold faster ORR kinetics (15.6 mA cm−2 @ 0.85 V) than that of the commercial Pt/C counterpart. Indeed, we perform density functional theory (DFT) to find that the Fe is charged with an extra 0.1 e− through the axially coordinate N ligand, which significantly enhances the ability to activate O2 and enables an easier desorption of the crucial intermediate *OH on the Fe-N5 configuration over the conventional Fe-N4 structure. © 2024, The Authors. All rights reserved.

关键词： Density functional theory

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