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Bioceramic scaffolds with two-step internal/external modification of copper-containing polydopamine enhance antibacterial and alveolar bone regeneration capability

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Journal of zhejiang University-Science B(Biomedicine & Biotechnology) 2024年第1期25卷 65-82页

作者： Xiaojian JIANG Lihong LEI Weilian SUN Yingming WEI Jiayin HAN Shuaiqi ZHONG Xianyan YANG Zhongru GOU Lili CHEN department of Oral Medicine the Second Affiliated HospitalZhejiang University School of MedicineHangzhou310009China Bio-nanomaterials and Regenerative Medicine Research Division Zhejiang–California International Nanosystem InstituteZhejiang UniversityHangzhou310058China

Magnesium-doped calcium silicate(CS)bioceramic scaffolds have unique advantages in mandibular defect repair;however,they lack antibacterial properties to cope with the complex oral microbiome.Herein,for the first time,the CS scaffold was functionally modified with a novel copper-containing polydopamine(PDA(Cu^(2+)))rapid deposition method,to construct internally modified(*P),externally modified(@PDA),and dually modified(*P@PDA)scaffolds.The morphology,degradation behavior,and mechanical properties of the obtained scaffolds were evaluated in vitro.The results showed that the CS*P@PDA had a unique micro-/nano-structural surface and appreciable mechanical resistance.During the prolonged immersion stage,the release of copper ions from the CS*P@PDA scaffolds was rapid in the early stage and exhibited long-term sustained release.The in vitro evaluation revealed that the release behavior of copper ions ascribed an excellent antibacterial effect to the CS*P@PDA,while the scaffolds retained good cytocompatibility with improved osteogenesis and angiogenesis effects.Finally,the PDA(Cu^(2+))-modified scaffolds showed effective early bone regeneration in a critical-size rabbit mandibular defect model.Overall,it was indicated that considerable antibacterial property along with the enhancement of alveolar bone regeneration can be imparted to the scaffold by the two-step PDA(Cu^(2+))modification,and the convenience and wide applicability of this technique make it a promising strategy to avoid bacterial infections on implants.

关键词： Copper-containing polydopamine Modification Antibacterial property Bone regeneration Angiogenesis Bioceramic scaffold

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Ru-Ni alloy nanosheets as tandem catalysts for electrochemical reduction of nitrate to ammonia

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Nano Research 2024年第6期17卷 4815-4824页

作者： Xingchao You Jiawei Xu Zechao Zhuang Junkai Xia Suwen Wang Haiyan Wei Yongfu Li Yanjiang Cai Hai Xiang Bing Yu State Key Laboratory of Subtropical Silviculture Zhejiang A&F UniversityHangzhou 311300China Ecological-Environment&Health College(EEHC) Zhejiang A&F UniversityHangzhou 311300China Jiangsu Key Laboratory of Numerical Simulation of Large Scale Complex Systems and School of Chemistry and Materials Science Nanjing Normal UniversityNanjing 210023China department of Chemistry Tsinghua UniversityBeijing 100084China department of Chemical Engineering Columbia UniversityNew YorkNY 10027USA

Developing electrocatalysts that exhibit both high activity and ammonia selectivity for nitrate reduction is a significant and demanding challenge,primarily due to the complex nature of the multiple-electron reduction process involved.An encouraging approach involves coupling highly active precious metals with transition metals to enhance catalytic performance through synergy.Here,we report a ruthenium-nickel alloy catalyst with nanosheets(Ru-Ni NSs)structure that achieves a remarkable ammonia Faradaic efficiency of approximately 95.93%,alongside a yield rate of up to 6.11 g·h^(−1)·cm^(−2).Moreover,the prepared Ru-Ni NSs exhibit exceptional stability during continuous nitrate reduction in a flow reactor for 100 h,maintaining a Faradaic efficiency of approximately 90%and an ammonia yield of 37.4 mg·L^(−1)·h^(−1)using 0.05 M nitrate alkaline electrolyte.Mechanistic studies reveal that the catalytic process follows a two-step pathway,in which HONO serves as a migration intermediate.The presence of a partially oxidized Ru(002)surface enhances the adsorption of nitrate and facilitates the release of the migration intermediate by adjusting the strength of the electrostatic and covalent interactions between the adsorbate and the surface,respectively.On the other hand,the Ni(111)surface promotes the utilization of the migration intermediate and requires less energy for NH_(3)desorption.This tandem process contributes to a high catalytic activity of Ru-Ni NSs towards nitrate reduction.

关键词： alloy catalyst nitrate reduction ammonia synthesis Faradaic efficiency

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An extended micromechanical-based plastic damage model for understanding water effects on quasi-brittle rocks

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International Journal of Mining Science and Technology 2024年第3期34卷 289-304页

作者： Qiaojuan Yu Shigui Du Qizhi Zhu Zhanyou Luo Sili Liu Lunyang Zhao Institute of Rock Mechanics Ningbo UniversityNingbo 315211China Ningbo Key Laboratory of Energy Geostructure Ningbo UniversityNingbo 315211China College of Civil and Transportation Engineering Hohai UniversityNanjing 210098China College of Civil Engineering Jiangsu Open UniversityNanjing 210036China South china Institution of Geotechnical Engineering School of Civil Engineering and TransportationSouth China University of TechnologyGuangzhou 510641China

Water effects on the mechanical properties of rocks have been extensively investigated through experiments and numerical models.However,few studies have established a comprehensive link between the microscopic mechanisms of water-related micro-crack and the constitutive behaviors of rocks.In this work,we shall propose an extended micromechanical-based plastic damage model for understanding weakening effect induced by the presence of water between micro-crack’s surfaces on quasi-brittle rocks,based on the Mori-Tanaka homogenization and irreversible thermodynamics framework.Regarding the physical mechanism,water strengthens micro-crack propagation,which induces damage evolution during the pre-and post-stage,and weakens the elastic effective properties of rock matrix.After proposing a special calibration procedure for the determination of model parameters based on the laboratory compression tests,the proposed micromechanical-based model is verified by comparing the model predictions to the experimental results.The model effectively captures the mechanical behaviors of quasibrittle rocks subjected to the weakening effects of water.

关键词： Water Micro-crack Damage Micro-mechanics Constitutive model Cohesive force

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Accelerating Oxygen Electrocatalysis Kinetics on Metal-Organic Frameworks via Bond Length Optimization

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Nano-Micro Letters 2024年第9期16卷 279-290页

作者： Fan He Yingnan Liu Xiaoxuan Yang Yaqi Chen Cheng‑Chieh Yang Chung‑Li Dong Qinggang He Bin Yang Zhongjian Li Yongbo Kuang Lecheng Lei Liming Dai Yang Hou Key Laboratory of Biomass Chemical Engineering of Ministry of education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China Institute of zhejiang University-Quzhou Quzhou 324000People’s Republic of China Ningbo Institute of Materials Technology and Engineering Chinese Academy of SciencesNingbo 315201People’s Republic of China School of Biological and Chemical Engineering NingboTech UniversityNingbo 315100People’s Republic of China department of Physics Tamkang UniversityNew Taipei 25137TaiwanPeople’s Republic of China Australian Carbon Materials Centre(A‑CMC) School of Chemical EngineeringUniversity of New South WalesSydneyNSW 2051Australia

Metal-organic frameworks(MOFs)have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity,but the limited catalytic activity and stability has hampered their practical use in water splitting.Herein,we develop a bond length adjustment strategy for optimizing naphthalene-based MOFs that synthesized by acid etching Co-naphthalenedicarboxylic acid-based MOFs(donated as AE-CoNDA)to serve as efficient catalyst for water splitting.AE-CoNDA exhibits a low overpotential of 260 mV to reach 10 mA cm^(−2)and a small Tafel slope of 62 mV dec^(−1)with excellent stability over 100 h.After integrated AE-CoNDA onto BiVO_(4),photocurrent density of 4.3 mA cm^(−2)is achieved at 1.23 V.Experimental investigations demonstrate that the stretched Co-O bond length was found to optimize the orbitals hybridization of Co 3d and O 2p,which accounts for the fast kinetics and high activity.Theoretical calculations reveal that the stretched Co-O bond length strengthens the adsorption of oxygen-contained intermediates at the Co active sites for highly efficient water splitting.

关键词： Metal-organic frameworks Bond length adjustment Spin state transition Orbitals hybridization Water splitting

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Construction of a Cu@hollow TS-1 nanoreactor based on a hierarchical full-spectrum solar light utilization strategy for photothermal synergistic artificial photosynthesis

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Carbon Energy 2024年第2期6卷 25-36页

作者： Sixian Zhu Qiao Zhao Hongxia Guo Li Liu Xiao Wang Xiwei Qi Xianguang Meng Wenquan Cui Hebei Key Laboratory for Environment Photocatalytic and Electrocatalytic Materials College of Chemical EngineeringNorth China University of Science and TechnologyTangshanChina School of Materials Science and Engineering National Institute for Advanced MaterialsTKL of Metal and Molecule-Based Material ChemistryNankai UniversityTianjinChina Hebei Iron and Steel Laboratory TangshanChina

The artificial photosynthesis technology has been recognized as a promising solution for CO_(2) utilization.Photothermal catalysis has been proposed as a novel strategy to promote the efficiency of artificial photosynthesis by coupling both photochemistry and thermochemistry.However,strategies for maximizing the use of solar spectra with different frequencies in photothermal catalysis are urgently needed.Here,a hierarchical full-spectrum solar light utilization strategy is proposed.Based on this strategy,a Cu@hollow titanium silicalite-1 zeolite(TS-1)nanoreactor with spatially separated photo/thermal catalytic sites is designed to realize high-efficiency photothermal catalytic artificial photosynthesis.The space-time yield of alcohol products over the optimal catalyst reached 64.4μmol g−1 h−1,with the selectivity of CH3CH2OH of 69.5%.This rationally designed hierarchical utilization strategy for solar light can be summarized as follows:(1)high-energy ultraviolet light is utilized to drive the initial and difficult CO_(2) activation step on the TS-1 shell;(2)visible light can induce the localized surface plasmon resonance effect on plasmonic Cu to generate hot electrons for H2O dissociation and subsequent reaction steps;and(3)low-energy near-infrared light is converted into heat by the simulated greenhouse effect by cavities to accelerate the carrier dynamics.This work provides some scientific and experimental bases for research on novel,highly efficient photothermal catalysts for artificial photosynthesis.

关键词： artificial photosynthesis full spectrum nanoreactors photothermal catalysis

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Construction of electron rich Fe active sites by FeCu alloy anchoring on carbon nitride for photocatalytic nitrogen reduction

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Rare Metals 2024年第4期43卷 1570-1579页

作者： Gang Dong Cong Huang Fei-Yang Chen Xue-Qin Liu Zhen Li Xiao-Li Su Tao Zeng Yun-Xia Chen Yi-Huang Chen Yang Wang School of Materials Science and Engineering Jingdezhen Ceramic University Faculty of Materials Science and Chemistry China University of Geosciences College of Chemistry and Materials Engineering Wenzhou University

Given the clean and inexhaustible solar energy from solar light,photocatalytic ammonia synthesis is extremely appealing.However,high electron-hole recombination rates and insufficient active sites severely limited N2 photoreaction reduction.Herein,we designed and fabricated FeCu alloy nanoparticles anchored on carbon nitride nanosheets with excellent photocatalyt ic ammonia synthesis performance.As a coupler between Fe and carbon nitride,Cu promotes the separation of photogenerated charge carriers in carbon nitride under solar light irradiation,and renters the semiconductor a forceful electron donor for the Fe active sites.The accumulated electrons at Fe sites furtherly facilitated the adsorption and activation of the molecular nitrogen.Besides,the uniform dispersed FeCu alloy nanoparticles were on carbon nitride nanosheets enhanced the stability of photocataly tic nitrogen reduction reaction,making the artificial photocataly tic ammonia synthesis more sustainable for application.This work highlights that a direct electron transfer channel can be used to regulate the photochemical nitrogen fixation network.

关键词： Photocatalytic N 2 fixation Carbon nitride FeCu alloy Active sites Hydrogenation pathway

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Advanced cellulose-based materials toward stabilizing zinc anodes

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Science china Chemistry 2024年第5期67卷 1465-1484页

作者： Zhijiang Li Xiang Chen Rui Zhang Taoyi Shen Jianchao Sun Zhongce Hu Lin Li Lanlan Yang Hou-Yong Yu College of Textile Science and Engineering(International Institute of Silk) Zhejiang Sci-Tech UniversityHangzhou 310018China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials Donghua UniversityShanghai 201620China School of Environment and Material Engineering Yantai UniversityYantai 264005China Institute for Carbon Neutralization College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China

Rechargeable aqueous zinc metal batteries(RAZMBs) have received extensive attention for large-scale energy storage systems due to the merits of Zn anodes, including moderate volumetric and gravimetric energy density, low redox potential, abundant reserve, low cost and impressive intrinsic safety. However, Zn anodes suffer from a series of adverse reactions(dendrite growth,hydrogen evolution, and surface passivation) resulting in low Coulombic efficiency, large polarization, and unsatisfied cycling performance, which inevitably hinder the wide application of RAZMBs. To address the above issues, cellulose-based materials are widely used for Zn anode protection because of their unique physical and chemical properties and other advantages such as biocompatibility, non-toxicity, degradability and easy extraction. In order to better understand the current progress in cellulosebased materials for the Zn anode protection, we have classified and summarized the relevant literatures. In this review, we summarize and elaborate the causes of poor reversibility for Zn anodes, including dendrite formation, hydrogen evolution, and surface passivation. Subsequently, the effective strategies(anode interfacial engineering, gel electrolyte optimization, and separator modification) of cellulose-based materials toward stabilizing Zn anodes are overviewed. In the end, the existing challenges and prospects of cellulose-based materials in Zn anode protection are summarized to shed light on future work.

关键词： Zn anode cellulose anode interfacial engineering gel electrolyte optimization separator modification

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Modulation of High-Order Harmonic Generation from a Monolayer ZnO by Co-rotating Two-Color Circularly Polarized Laser Fields

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Chinese Physics Letters 2024年第1期41卷 34-38页

作者：乔月陈家祺周书山陈基根蒋士成杨玉军 School of Materials Science and Engineering Taizhou UniversityJiaojiang 318000China Institute of Atomic and Molecular Physics Jilin UniversityChangchun 130012China Jilin Provincial Key Laboratory of Applied Atomic and Molecular Spectroscopy(Jilin University) Changchun 130012China School of Physics and Electronic Technology Liaoning Normal UniversityDalian 116029China State Key Laboratory of Precision Spectroscopy East China Normal UniversityShanghai 200062China

By numerically solving the two-dimensional semiconductor Bloch equation,we study the high-order harmonic emission of a monolayer ZnO under the driving of co-rotating two-color circularly polarized laser pulses.By changing the relative phase between the fundamental frequency field and the second one,it is found that the harmonic intensity in the platform region can be significantly modulated.In the higher order,the harmonic intensity can be increased by about one order of magnitude.Through time-frequency analysis,it is demonstrated that the emission trajectory of monolayer ZnO can be controlled by the relative phase,and the harmonic enhancement is caused by the second quantum trajectory with the higher emission probability.In addition,near-circularly polarized harmonics can be generated in the co-rotating two-color circularly polarized fields.With the change of the relative phase,the harmonics in the platform region can be altered from left-handed near-circularly polarization to right-handed one.Our results can obtain high-intensity harmonic radiation with an adjustable ellipticity,which provides an opportunity for syntheses of circularly polarized attosecond pulses.

关键词： polarization rotating harmonic

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Reinforced Lewis covalent bond by twinborn nitride heterostructure for lithium-sulfur batteries

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Journal of Energy Chemistry 2024年第1期88卷 363-372,I0009页

作者： Yaochen Song Pengkai Tang Yanjie Wang Yi Wang Linnan Bi Qi Liang Liang He Qingyu Xie Yiyong Zhang Peng Dong Yingjie Zhang Yao Yao Jiaxuan Liao Sizhe Wang Yangtze Delta Region Institute(QuZhou) University of Electronic Science and Technology of ChinaQinzhou 324000ZhejiangChina School of Materials and Energy University of Electronic Science and Technology of ChinaChengdu 611731SichuanChina National and Local Joint Engineering Laboratory for Lithium-ion Batteries and Materials Preparation Technology Key Laboratory of Advanced Battery Materials of Yunnan ProvinceFaculty of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunming 650093YunnanChina School of Materials Science and Engineering Shaanxi Key Laboratory of Green Preparation and Functionalization for Inorganic MaterialsShaanxi University of Science&TechnologyXi’an 710021ShaanxiChina School of Environmental Science and Engineering North China Electric Power UniversityBaoding 071003HebeiChina

The practical application of lithium-sulfur(Li-S)batteries,as promising next-generation batteries,is hindered by their shuttle effect and the slow redox kinetics.Herein,a tungsten and molybdenum nitride heterostructure functionalized with hollow metal-organic framework-derived carbon(W_(2)N/Mo_(2)N)was proposed as the sulfur host.The hollow spherical structure provides storage space for sulfur,enhances electrical conductivity,and inhibits volume expansion.The metal atoms in the nitrides bonded with lithium polysulfides(Li PSs)through Lewis covalent bonds,enhancing the high catalytic activity of the nitrides and effectively reducing the energy barrier of Li PSs redox conversion.Moreover,the high intrinsic conductivity of nitrides and the ability of the heterostructure interface to accelerate electron/ion transport improved the Li+transmission.By leveraging the combined properties of strong adsorption and high catalytic activity,the sulfur host effectively inhibited the shuttle effect and accelerated the redox kinetics of Li PSs.High-efficiency Li+transmission,strong adsorption,and the efficient catalytic conversion activities of Li PSs in the heterostructure were experimentally and theoretically verified.The results indicate that the W_(2)N/Mo_(2)N cathode provides stable,and long-term cycling(over 2000 cycles)at 3 C with a low attenuation rate of 0.0196%per cycle.The design strategy of a twinborn nitride heterostructure thus provides a functionalized solution for advanced Li-S batteries.

关键词： Heterostructure Adsorption Redox kinetics

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下颌第一磨牙远舌根的存在与牙周状态的临床相关性分析：一项采用锥形射束电脑断层扫描分析的横断面研究（英文）

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Journal of zhejiang University-Science B(Biomedicine & Biotechnology) 2024年第3期 244-255页

作者：茅飞飞王萌周帅赵妍黄佳萍尹凤英杨海萍丁佩惠浙江大学医学院附属口腔医院浙江大学口腔医学院浙江省口腔疾病临床医学研究中心浙江省口腔生物医学研究重点实验室浙江大学癌症研究所

下颌第一磨牙远舌根已经被广泛报道，它的存在使牙周炎的治疗更为复杂。本研究旨在评估中国东部地区人群中下颌第一磨牙远舌根的发生率，并探讨远舌根的形态学特征与骨破坏及牙周状况的关联性。本研究通过对中国东部地区836例患者共149... 详细信息

下颌第一磨牙远舌根已经被广泛报道，它的存在使牙周炎的治疗更为复杂。本研究旨在评估中国东部地区人群中下颌第一磨牙远舌根的发生率，并探讨远舌根的形态学特征与骨破坏及牙周状况的关联性。本研究通过对中国东部地区836例患者共1497颗下颌第一磨牙的锥形射束电脑断层扫描（CBCT）进行流行病学分析。其中，69例患者的103颗下颌第一磨牙有完整的牙周检查表。随后采用相关分析和回归分析评估下颌第一磨牙远舌根的形态学特征与骨缺损及牙周临床参数间的关系，包括临床附着缺失、探诊深度、牙龈退缩和根分叉病变情况。研究结果发现，中国东部地区人群中下颌第一磨牙远舌根在患者和牙位水平的患病率分别为29.4%和26.3%。多元线性回归分析表明，第一磨牙舌侧的骨缺损及临床附着丧失水平与位于横截面的远舌根与近中根的分离角呈负相关，而与年龄和位于冠状面上的远颊根与近中根的分离角呈正相关。综上，中国东部地区人群下颌第一磨牙远舌根患病率较高，而且下颌第一磨牙远舌根的形态特征与牙周状况具有相关性。本研究旨在提高下颌第一磨牙远舌根的早期诊断率，并对存在远舌根的第一磨牙的治疗决策提供重要的信息。

关键词：远舌根下颌第一磨牙牙周临床参数临床附着丧失锥形射束电脑断层扫描(CBCT)

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