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Controllable selective anchoring of subnanometric Ru clusters or single-atoms/clusters on tungsten nitride for the hydrogen oxidation

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science china Chemistry 2024年第11期67卷 3749-3756页

作者： Qijiao Sun Chuanqiang Wu Yiqiang Sun Yuan Shen Lei Zhao Xiaodong Yang li Yang Yunxiang lin Keke Mao Kun Xu school of Chemistry and Chemical engineering Key Laboratory of Functional Inorganic Material Chemistry of Anhui Province Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education Anhui University Information materials and Intelligent Sensing Laboratory of Anhui Province Institutes of Physical Science and Information TechnologyAnhui University school of Chemistry and Chemical engineering University of Jinan school of Energy and Environment Anhui University of Technology

The impregnation method in the preparation of metal cluster catalysts typically inadvertently introduces single atoms（SAs） into the substrate. However, the question of whether the introduction of SAs will further improve the catalytic activity of cluster systems for specific reactions such as the hydrogen oxidation reaction（HOR） remains unraveled. Herein, we demonstrate Ru clusters anchored on WN nanowires（RuC/WN） show a higher alkaline HOR catalytic activity in comparison with Ru SAs and nanoclusters（NCs）-coupled catalyst anchored on WN nanowires system（RuC,S/WN）. Notably, the RuC/WN exhibits superb intrinsic catalytic activity with a mass-normalized exchange current density of 890 m A mg-1PGM, which is among the top level of well developed Ru-based HOR catalysts. Both theoretical simulation and experimental investigation suggest that RuC/WN owns an optimized H*and OH*reaction intermediates for the alkaline HOR, therefore resulting in the excellent intrinsic HOR catalytic performance.

关键词： hydrogen oxidation reaction Ru cluster catalyst Ru single atoms and nanoclusters coupled catalyst tungsten nitride substrate

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Approaching Ultimate Synthesis Reaction Rate of Ni-Rich Layered Cathodes for lithium-Ion Batteries

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Nano-Micro Letters 2024年第10期16卷 392-402页

作者： Zhedong liu Jingchao Zhang Jiawei luo Zhaoxin Guo Haoran Jiang Zekun li Yuhang liu Zijing Song Rui liu Wei-Di liu Wenbin Hu Yanan Chen school of materials science and engineering Tianjin UniversityTianjin 300072People's Republic of China school of materials science and engineering Shandong University of Science and TechnologyQingdao 266590People's Republic of China Australian Institute of Bioengineering and Nanotechnology The University of QueenslandSt LuciaQLD 4072Australia

Nickel-rich layered oxide liNi_(x)Co_(y)MnzO_(2)(NCM,x+y+z=1)is the most promising cathode material for high-energy lithium-ion ***,conventional synthesis methods are limited by the slow heating rate,sluggish reaction dynamics,high energy consumption,and long reaction *** overcome these chal-lenges,we first employed a high-temperature shock(HTS)strategy for fast synthesis of the NCM,and the approaching ultimate reaction rate of solid phase transition is deeply investigated for the first *** the HTS process,ultrafast average reaction rate of phase transition from Ni_(0.6)Co_(0.2)Mn_(0.2)(OH)_(2) to li-containing oxides is 66.7(%s^(-1)),that is,taking only 1.5 *** ultrahigh heating rate leads to fast reaction kinetics,which induces the rapid phase transition of NCM *** HTS-synthesized nickel-rich layered oxides perform good cycling performances(94%for NCM523,94%for NCM622,and 80%for NCM811 after 200 cycles at 4.3 V).These findings might also assist to pave the way for preparing effectively Ni-rich layered oxides for lithium-ion batteries.

关键词： Nickel-rich layered oxides High-temperature shock Solid reaction kinetics Phase transition Reaction rate

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以阳离子Gemini表面活性剂C_(12-2-12)为模板合成纯硅立方介孔材料

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山东大学学报（理学版） 2004年第3期39卷 80-83页

作者：许军韩书华侯万国党文修闫欣王仁亮孙立新山东大学胶体与界面化学教育部重点实验室山东济南250100 山东大学化学与化工学院山东济南250100

用Germini表面活性剂[C12H25N+(CH3)2-(CH2)2-N+(CH3)2C12H25]·2Br-作模板合成了立方结构的介孔二氧化硅,并且用小角X射线衍射和氮气吸附-脱附技术对样品进行了表征.结果表明,所得到的介孔二氧化硅为立方结构,晶胞参数在8.45-8.57 nm之... 详细信息

用Germini表面活性剂[C12H25N+(CH3)2-(CH2)2-N+(CH3)2C12H25]·2Br-作模板合成了立方结构的介孔二氧化硅,并且用小角X射线衍射和氮气吸附-脱附技术对样品进行了表征.结果表明,所得到的介孔二氧化硅为立方结构,晶胞参数在8.45-8.57 nm之间;孔道的有序性随表面活性剂与Na2SiO3比例的增大而增加.氮气吸附-脱附等温线为第Ⅳ类型的等温线,在相对压力p/p0=0.15-0.25和P/p0=0.8-1的范围内出现两个H1型滞后环,分别是由介孔孔道和颗粒之间的空穴引起的.BET表面积也随表面活性剂与Na2SiO3比例的增大而增大,最大可达1 100m2/g,最可几孔径在2.20 nm左右.

关键词：阳离子Gemini表面活性剂立方介孔材料模板

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Enhancement of CH_(3)CO^(*) adsorption by editing d-orbital states of Pd to boost C–C bond cleavage of ethanol eletrooxidation

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science china Chemistry 2024年第2期67卷 696-704页

作者： Yuchen Qin Fengqi Wang Pei liu Jinyu Ye Qian Wang Yao Wang Guangce Jiang lijie liu Pengfang Zhang Xiaobiao liu Xin Zheng Yunlai Ren Junjun li Zhicheng Zhang College of sciences Henan Agricultural UniversityZhengzhou450000China Tianjin Key Laboratory of Molecular Optoelectronic sciences Department of ChemistrySchool of ScienceTianjin University&Collaborative Innovation Center of Chemical Science and EngineeringTianjin300072China College of Chemistry and Chemical engineering Xiamen UniversityXiamen361005China Department of Analysis Sinopec Engineering Group Luoyang R&D Center of TechnologyLuoyang471000China school of Chemical and material engineering Jiangnan UniversityWuxi214211China shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell technology Liaocheng UniversityLiaocheng252000China

Improving the complete ethanol electrooxidation on Pd-based catalysts in alkaline media has drawn widely attention due to the high mass energy ***,the weak adsorption energy of CH_(3)CO^(*) on Pd restricts the C–C bond *** by the molecular orbital theory,we proposed the d-state-editing strategy to construct more unoccupied d-states of Pd for the enhanced interaction with CH_(3)CO^(*) to break C–C *** expected,the reduced number of e_g electrons and more unoccupied d-states of Pd successfully formed on as-prepared porous Rh Au–Pd Cu nanosheets(PNSs).Theoretical calculations show that the optimized d-states of Rh Au–Pd Cu PNS can effectively improve the adsorption of CH_(3)CO^(*) and drastically reduce the energy barrier of C–C bond cleavage,thus boosting the complete oxidation of *** charge ratio of C_1 pathway on Rh Au–Pd Cu PNSs is 51.5%,more than 2 times higher than that of Pd *** finding provides an innovative perspective for the design of highly-efficient noble-based electrocatalysts.

关键词： C–C bond cleavage CH_(3)CO^(*)adsorption unoccupied d-states ethanol oxidation reaction RhAu–PdCu porous nanosheets

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MXene Sediment-Based Poly(vinyl alcohol)/Sodium Alginate Aerogel Evaporator with Vertically Aligned Channels for Highly Efficient Solar Steam Generation

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Nano-Micro Letters 2024年第10期16卷 638-654页

作者： Tian Wang Meng li Hongxing Xu Xiao Wang Mingshu Jia Xianguang Hou Shuai Gao Qingman liu Qihang Yang Mingwei Tian lijun Qu Zhenhua Song Xiaohu Wu lili Wang Xiansheng Zhang shandong Key Laboratory of Medical and Health Textile materials College of Textiles and ClothingState Key Laboratory of Bio-Fibers and Eco-TextilesResearch Center for Intelligent and Wearable TechnologyQingdao UniversityQingdao 266071People's Republic of China Department of Pharmacology Qingdao University School of PharmacyQingdao UniversityQingdao 266071People's Republic of China shandong Institute of Advanced technology Jinan 250100People's Republic of China College of Electromechanical engineering Qingdao University of Science and TechnologyQingdao 266061People's Republic of China

Solar-driven interfacial evaporation from seawater is considered an effective way to alleviate the emerging freshwater crisis because of its green and environmentally friendly ***,developing an evaporator with high efficiency,stability,and salt resistance remains a key ***,with an internal photothermal conversion efficiency of 100%,has received tremendous research interest as a photothermal ***,the process to prepare the MXene with monolayer is inefficient and generates a large amount of“waste”MXene sediments(MS).Here,MXene sediments is selected as the photothermal material,and a three-dimensional MXene sediments/poly(vinyl alcohol)/sodium alginate aerogel evaporator with vertically aligned pores by directional freezing method is innovatively *** vertical porous structure enables the evaporator to improve water transport,light capture,and high evaporation *** swabs and polypropylene are used as the water channel and support,respectively,thus fabricating a self-floating *** evaporator exhibits an evaporation rate of 3.6 kg m^(-2)h^(-1)under one-sun illumination,and 18.37 kg m^(-2)of freshwater is collected in the condensation collection device after 7 h of outdoor sun *** evaporator also displays excellent oil and salt *** research fully utilizes“waste”MS,enabling a self-floating evaporation device for freshwater collection.

关键词： MXene sediments Porous structure Desalination Self-floating

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Revisiting N,S co-doped carbon materials with boosted electrochemical performance in sodium-ion capacitors:The manipulation of internal electric field

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Nano Research Energy 2024年第1期3卷 10-18页

作者： Shuli li Jinqiang Zhang Yanan li Pengxiang Fan Mingbo Wu shandong Institute of Petroleum and Chemical technology Dongying 257000China school of Chemical engineering The University of AdelaideNorth TerraceAdelaideSA 5005Australia State key laboratory of Heavy Oil Processing Institute of New EnergyCollege of Chemical EngineeringChina University of Petroleum(East China)Qingdao 266580China shandong Hi-tech Spring material technology Co. Ltd.Dongying 257000China

Heteroatom doping has emerged as a prevailing strategy to enhance the storage of sodium ions in carbon ***,the underlying mechanism governing the performance enhancement remains ***,we fabricated N/S co-doped carbon beaded fibers(S-N-CBFs),which exhibited glorious rate performance and durableness in Na+storage,showcasing no obvious capacity decay even after 3500 ***,when used as anodes in sodium-ion capacitors,the S-N-CBFs delivered exceptional results,boasting a high energy density of 225 Wh·kg^(-1),superior power output of 22500 W·kg^(-1),and outstanding cycling stability with a capacity attenuation of merely 0.014%per cycle after 4000 cycles at 2 A·g^(-1).Mechanistic investigations revealed that the incorporation of both pyridinic N and pyrrolic N into the carbon matrix of S-N-CBFs induced internal electric fields(IEFs),with the former IEF being stronger than the latter,in conjunction with the doped S *** functional theory calculations further unveiled that the intensity of the IEF directly influenced the adsorption of Na+,thereby resulting in the exceptional performances of S-N-CBFs as sodium-ion storage *** work uncovers the pivotal role of IEF in regulating the electronic structure of carbon materials and enhancing their Na^(+)storage capabilities,providing valuable insights for the development of more advanced electrode materials.

关键词： N/S co-doped carbon internal electric field Na^(+)adsorption sodium-ion storage sodium-ion capacitors

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Phosphorus-doped iron-nitrogen-carbon catalyst with pentacoordinated single atom sites for efficient oxygen reduction

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Nano Research 2023年第2期16卷 1810-1819页

作者： lili Fan Xiaofei Wei Xuting li Zhanning liu Mengfei li Shuo liu Zixi Kang Fangna Dai Xiaoqing lu Daofeng Sun school of materials science and engineering China University of Petroleum(East China)Qingdao 266580China College of science China University of Petroleum(East China)Qingdao 266580China

Single-atomic Fe-N4 is the well-acknowledged active site in iron-nitrogen-carbon(Fe-N-C)material for oxygen reduction reaction(ORR).The adjusting of the electronic distribution of Fe-N4 is promising for further enhancing the performance of the Fe-N-C ***,a phosphorus(P)-doped Fe-N-C catalyst with penta-coordinated single atom sites(FeNPC)is reported for efficient oxygen *** K-edge X-ray absorption spectroscopy(XAS)verifies the coordination environment of single Fe atom,while density functional theory(DFT)calculations reveal that the penta-coordination and neighboring doped P atoms can simultaneously change the electronic distribution of Fe-N_(4)and its adsorption strength of key intermediates,reducing the reactionfree energy of the potential-limiting *** tests validate the remarkable intrinsic ORR activity of FeNPC in alkaline media(a half-wave potential(E_(1/2))of 0.904 V *** hydrogen electrode(RHE)and limited current density(JL)of 6.23 mA·cm^(−2))and an enhanced ORR performance in neutral(E_(1/2)=0.751 V,J_(L)=5.27 mA·cm^(−2))and acidic media(E_(1/2)=0.735 V,JL=5.82 mA·cm^(−2))with excellent stability,highlighting the benefits of optimizing the local environment of singleatomic Fe-N4.

关键词： Fe-N-C Fe-N4 penta-coordination oxygen reduction reaction P-doping

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Significantly enhanced ion-migration and sodium-storage capability derived by strongly coupled dual interfacial engineering in heterogeneous bimetallic sulfides with densified carbon matrix

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SusMat 2024年第3期4卷 175-191页

作者： Wenxi Zhao Xiaoqing Ma Guangzhao Wang linglin Tan Xinqin Wang Xun He Yan Wang Yongsong luo Dongdong Zheng Shengjun Sun Qian liu luming li Wei Chu Xuping Sun school of Electronic Information engineering Yangtze Normal UniversityFulingChongqingChina Institute of Fundamental and Frontier sciences University of Electronic Science and Technology of ChinaChengduSichuanChina school of Electronic engineering Lanzhou City UniversityLanzhouGansuChina College of Chemistry Chemical Engineering and Materials ScienceShandong Normal UniversityJinanShandongChina Institute for Advanced Study Chengdu UniversityChengduSichuanChina

The development of highly efficient sodium-ion batteries depends critically on the successful exploitation of advanced anode hosts that is capable of overcoming sluggish reaction kinetics while also withstanding severe structural deformation triggered by the large radius of Na^(+)-***,a hierarchically hybrid material with hetero-Co_(3)S_(4)/NiS hollow nanosphere packaged into a densified N-doped carbonmatrix(Co_(3)S_(4)/NiS@N-C)was designed and fabricated utilizing CoNi-glycerate as the self-sacrifice template,making the utmost of the synergistic effect of hetero-Co_(3)S_(4)/NiS with strong electric field and rich reaction active-sites together with the densified outer-carbon scaffolds with remarkable electronic conductivity and robust mechanical *** anticipated,as-fabricated Co_(3)S_(4)/NiS@N-C anode affords remarkable specific capacity,prolonged cycle lifespan up to 2400 cycles with an only 0.05%fading each cycle at 20.0 A g^(−1),and excellent rate feature(354.9 mAh g^(−1)at 30.0 A g^(−1)),one of the best performances for most existing Co_(3)S_(4)/NiS-based *** situ structural characterizations in tandem with theoretical analysis demonstrate the reversible insertion-conversion mechanism of initially proceeding with Na^(+)de-/intercalation and superior heterogeneous interfacial reaction behavior with strong Na^(+)-adsorption ***,sodium-ion full cell and hybrid capacitor based on Co_(3)S_(4)/NiS@N-C anode exhibit impressive electrochemical characteristics on cycling performance and rate capability,showcasing its outstanding feasibility toward practical use.

关键词： anode materials bimetallic metal sulfides heterogeneous interface outer-carbon skeleton sodium ion battery

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碱金属修饰的萘炔/萘二炔对CO_(2)选择性吸附分离的理论计算

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无机化学学报 2024年第3期40卷 515-522页

作者：赵杰刘森殷齐康鲁效庆王兆杰管网集团(新疆)联合管道有限责任公司乌鲁木齐830000 中国石油大学(华东)材料科学与工程学院青岛266580

采用巨正则蒙特卡洛模拟和密度泛函理论结合的方式探究了不同碱金属(alkali metal,AM,包括li、Na、K)修饰提升萘炔(naphyne,NY)和萘二炔(naphdiyne,NDY)的CO_(2)吸附分离性能。通过结合能和结构的电子性质分析发现,AM修饰的NY和NDY具有... 详细信息

采用巨正则蒙特卡洛模拟和密度泛函理论结合的方式探究了不同碱金属(alkali metal,AM,包括li、Na、K)修饰提升萘炔(naphyne,NY)和萘二炔(naphdiyne,NDY)的CO_(2)吸附分离性能。通过结合能和结构的电子性质分析发现,AM修饰的NY和NDY具有良好的结构稳定性。在298 K、100 k Pa的条件下,li修饰的萘二炔(li-NDY)表现出高达11.37 mmol·g^(-1)的CO_(2)吸附量和430.85的CO_(2)选择性(优于N_(2))。同时,利用气体吸附密度分布揭示了不同AM修饰的NY/NDY(AM-NY、AM-NDY)具有高吸附量的原因,以及二者作用效果差异的本质。最后,从吸附热、库仑和范德瓦耳斯相互作用等角度详细说明了AM引入的改性机制。

关键词：二维碳材料 CO_(2)吸附分离密度泛函理论巨正则蒙特卡洛

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微发酵调理牛排制备工艺优化及品质特性研究

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食品与生物技术学报 2024年第6期43卷 95-103页

作者：朱丽君张永东陆香楠余群力韩广星李航甘肃农业大学食品科学与工程学院甘肃兰州730030 张掖市畜牧兽医工作站甘肃张掖734099 山东绿润食品有限公司山东临沂276000 重庆恒都农业集团有限公司重庆408200

选取牛腿肉为原料,通过预试验筛选,确定以戊糖片球菌和乳酸片球菌混合菌为发酵剂,采用响应面法优化调理牛排制备发酵工艺,以低温静腌10.00 h未发酵调理牛排为对照,测定不同处理组对牛排pH、质构、色度和风味的影响,并采用模糊综合评判... 详细信息

选取牛腿肉为原料,通过预试验筛选,确定以戊糖片球菌和乳酸片球菌混合菌为发酵剂,采用响应面法优化调理牛排制备发酵工艺,以低温静腌10.00 h未发酵调理牛排为对照,测定不同处理组对牛排pH、质构、色度和风味的影响,并采用模糊综合评判法对其感官品质进行评价。结果表明,微发酵调理牛排最优工艺条件为:发酵剂添加质量分数0.015%,发酵时间10.00 h,发酵温度31.5℃。与未发酵调理牛排相比,微发酵调理牛排pH、硬度和咀嚼性显著降低(P<0.05),L^(*)值、a^(*)值、b^(*)值和感官评分显著升高(P<0.05),调理牛排发酵后酯类、醛类、酮类、烯烃类及其他化合物种类分别增加了0.4%、3.0%、0.7%、0.5%和0.7%。综上,微发酵可以改善牛排嫩度和风味,提高产品品质,为牛排嫩化和发酵产品的创新研究提供了依据。

关键词：微发酵调理牛排工艺优化理化特性风味感官评价

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