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Self-supported NiFe-LDH nanosheets on NiMo-based nanorods as high-performance bifunctional electrocatalysts for overall water splitting at industrial-level current densities

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Nano Research 2024年第5期17卷 3769-3776页

作者： Yan Zhang Biao Feng MingLei Yan Zhen Shen Yiqun Chen Jingyi Tian Fengfei Xu Guanghai Chen xizhang wang Lijun Yang Qiang Wu Zheng Hu Key Laboratory of Mesoscopic Chemistry of Ministry of Education(MOE)and Jiangsu Provincial Lab for Nanotechnology School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China College of Water Conservancy and Hydropower Engineering Sichuan Agricultural UniversityYa’an 625014China

Efficient,durable and economic electrocatalysts are crucial for commercializing water electrolysis ***,we report an advanced bifunctional electrocatalyst for alkaline water splitting by growing NiFe-layered double hydroxide(NiFe-LDH)nanosheet arrays on the conductive NiMo-based nanorods deposited on Ni foam to form a three-dimensional(3D)architecture,which exhibits exceptional performances for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In overall water splitting,only the low operation voltages of 1.45/1.61 V are required to reach the current density of 10/500 mA·cm^(-2),and the continuous water splitting at an industrial-level current density of 500 mA·cm^(-2) shows a negligible degradation(1.8%)of the cell voltage over 1000 *** outstanding performance is ascribed to the synergism of the HER-active NiMo-based nanorods and the OER-active NiFe-LDH nanosheet arrays of the hybridized 3D ***,the dense NiFe-LDH nanosheet arrays enhance the local pH on cathode by retarding OH-diffusion and enlarge the electrochemically active surface area on anode,while the conductive NiMo-based nanorods on Ni foam much decrease the charge-transfer resistances of both *** study provides an efficient strategy to explore advanced bifunctional electrocatalysts for overall water splitting by rationally hybridizing HER-and OER-active components.

关键词： alkaline water splitting bifunctional electrocatalysts layered double hydroxides high durability industrial current densities

Impact of Pd single-site coordination structure on catalytic performance for semihydrogenation of acetylene

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Nano Research 2024年第9期17卷 8243-8249页

作者： Yu Zeng Minqi Xia Fujie Gao Changkai Zhou Xueyi Cheng Liwei Liu Liu Jiao Qiang Wu xizhang wang Lijun Yang Yining Fan Zheng Hu Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Laboratory for Nanotechnology School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Semihydrogenation of trace acetylene in an ethylene gas stream is a vital step for the industrial production of polyethylene,in which Pd single-site catalysts(SSCs)have great ***,two Pd SSCs with different coordination structures are prepared on hierarchical nitrogen-doped carbon nanocages(hNCNC)by regulating the nitrogen species with or without using *** using dicyandiamide,the obtained Pd1-Ndicy/hNCNC SSC features the coordinated Pd by two pyridinic N and two pyrrolic N(PdN^(py)_(2)N^(pr)_(2)).Without using dicyandiamide,the obtained Pd1/hNCNC SSC features the coordinated Pd by pyridinic N and C(PdN^(py_(x)C_(4-x)),x=1-4).The former exhibits an 18-fold increase in catalytic activity compared to the *** results reveal the abundant unoccupied orbital states above the Fermi level of moiety,which can facilitate the activation of substrate molecules and dynamics of acetylene hydrogenation as supported by the combined theoretical and experimental *** addition,PdN^(py)_(2)N^(pr)_(2)the moiety presents a favorable desorption of ***,the Pd1-Ndicy/hNCNC SSC exhibits high C2H2 conversion(99%)and C2H4 selectivity(87%)at 160℃.This study demonstrates the impact of Pd single-site coordination structure on catalytic performance,which is significant for the rational design of advanced Pd SSCs on carbon-based supports.

关键词： coordination structure hierarchical nitrogen-doped carbon nanocages palladium semihydrogenation of acetylene singlesite catalysts

Mesostructured carbon-based nanocages: an advanced platform for energy chemistry

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Science China Chemistry 2020年第5期63卷 665-681页

作者： Qiang Wu Lijun Yang xizhang wang Zheng Hu Key Laboratory of Mesoscopic Chemistry of Ministry of Education School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

The electrochemistry in energy conversion and storage(ECS) not only relies on the active species in catalysts or energy-storage materials, but also involves mass/ion transport around the active species and electron transfer to the external circuit. To realize high-rate ECS process, new architectures for catalysts or energy-storage electrodes are required to ensure more efficient mass/charge transport. 3 D porous mesostructured materials constructed by nanoscale functional units can form a continuous conductive network for electron transfer and an interconnected multiscale pores for mass/ion transport while maintaining the high surface area, showing great promise in boosting the ECS process. In this review, we summarize the recent progress on the design,construction and applications of 3 D mesostructured carbon-based nanocages for ECS. The role of the hierarchical architectures to the high rate performance is discussed to highlight the merits of the mesostructured materials. The perspective on future opportunities and challenges is also outlined for deepening and extending the related studies and applications.

关键词： carbon-based nanocages mesostructures energy conversion and storage enhanced mass/charge transport multifunction platform

Defect-induced deposition of manganese oxides on hierarchical carbon nanocages for high-performance lithium-oxygen batteries

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Nano Research 2022年第5期15卷 4132-4136页

作者： Baoxing wang Chenxia Liu Lijun Yang Qiang Wu xizhang wang Zheng Hu Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Laboratory for Nanotechnology School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

The cathode of lithium-oxygen(Li-O_(2))batteries should have large space for high Li_(2)O_(2) uptake and superior electrocatalytic activity to oxygen evolution/reduction for long ***,a high-performance MnO_(x)/hCNC cathode was constructed by the defect-induced deposition of manganese oxide(MnOx)nanoparticles on hierarchical carbon nanocages(hCNC).The corresponding Li-O2 battery(MnOx/hCNC@Li-O_(2))exhibited excellent electrocatalytic activity with the low overpotential of 0.73-0.99 V in the current density range of 0.1-1.0 A·g^(-1).The full discharge capacity and cycling life of MnO_(x)/hCNC@Li-O_(2) were increased by~86.7%and~91%,respectively,compared with the hCNC@Li-O_(2) *** superior performance of MnO_(x)/hCNC cathode was ascribed to(i)the highly dispersed MnO_(x) nanoparticles for boosting the reversibility of oxygen evolution/reduction reactions,(ii)the interconnecting pore structure for increasing Li_(2)O_(2) accommodation and facilitating charge/mass transfer,and(iii)the concealed surface defects of hCNC for suppressing side *** study demonstrated an effective strategy to improve the performance of Li-O_(2) batteries by constructing cathodes with highly dispersed catalytic sites and hierarchical porous structure.

关键词： Li-O_(2) batteries hierarchical carbon nanocages manganese oxide electrocatalysis defect-induced deposition

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超高压技术在果品加工中的应用研究进展

食品研究与开发 2024年第2期45卷 212-217页

作者：胡爱军王威于作昌王玺章于敏燕山东鲁海食品有限公司山东莱阳265224 天津科技大学食品科学与工程学院天津300457

超高压技术是一种绿色非热加工技术,不仅能用于果品杀菌,还能最大限度地保持加工果品的营养物质,获得高质量的产品。该文综述超高压对果品感官品质、理化性质、营养成分、酶活力、生物活性物质以及微生物的影响,并指出超高压技术处理果... 详细信息

超高压技术是一种绿色非热加工技术,不仅能用于果品杀菌,还能最大限度地保持加工果品的营养物质,获得高质量的产品。该文综述超高压对果品感官品质、理化性质、营养成分、酶活力、生物活性物质以及微生物的影响,并指出超高压技术处理果品存在的问题及未来发展的方向,可为超高压技术在果品加工中的应用提供参考。

关键词：超高压果品理化性质微生物感官特性

Boosting faradaic efficiency of CO_(2)electroreduction to CO for Fe-NC single-site catalysts by stabilizing Fe^(3+)sites via F-doping

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Nano Research 2022年第9期15卷 7896-7902页

作者： Yiqun Chen Guochang Li Yu Zeng Lijie Yan xizhang wang Lijun Yang Qiang Wu Zheng Hu Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for Nanotechnology School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

The atomically dispersed Fe^(3+)sites of Fe-N-C single-site catalysts(SSCs)are demonstrated as the active sites for CO_(2)electroreduction(CO_(2)RR)to CO but suffer from the reduction to Fe^(2+)at~−0.5 V,accompanied by the drop of CO faradaic efficiency(FECO)and deterioration of partial current(JCO).Herein,we report the construction of F-doped Fe-N-C SSCs and the electron-withdrawing character of fluorine could stabilize Fe3+sites,which promotes the FECO from the volcano-like highest value(88.2%@−0.40 V)to the high plateau(>88.5%@−0.40-−0.60 V),with a much-increased JCO(from 3.24 to 11.23 mA·cm^(−2)).The enhancement is ascribed to the thermodynamically facilitated CO_(2)RR and suppressed competing hydrogen evolution reaction,as well as the kinetically increased electroactive surface area and improved charge transfer,due to the stabilized Fe^(3+)sites and enriched defects by fluorine *** finding provides an efficient strategy to enhance the CO_(2)RR performance of Fe-N-C SSCs by stabilizing Fe^(3+).

关键词： carbon dioxide electroreduction iron-nitrogen-carbon single-site catalysts fluorine-doping active site regulation

Micro–meso-macroporous FeCo-N-C derived from hierarchical bimetallic FeCo-ZIFs as cathode catalysts for enhanced Li-O2 batteries performance

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Journal of Energy Chemistry 2019年第8期28卷 212-219,I0008页

作者： Fufang Chao Baoxing wang Jiaojiao Ren Yingwei Lu Wenrui Zhang xizhang wang Lin Cheng Yongbing Lou Jinxi Chen School of Chemistry and Chemical Engineering Jiangsu Engineering Laboratory of Smart Carbon-Rich Materials and Device Southeast UniversityNanjing 211189 Jiangsu China Key Laboratory of Mesoscopic Chemistry of MOE Jiangsu Provincial Lab for Nanotechnology School of Chemistry and Chemical Engineering Nanjing UniversityNanjing 210093 Jiangsu China

Developing bifunctional catalysts that increase both the OER and ORR kinetics and transport reactants with high efficiency is desirable. Herein, micro–meso-macroporous FeCo-N-C-X(denoted as "MFeCo-N-C-X", X represents Fe/Co molar ratio in bimetallic zeolite imidazole frameworks FeCo-ZIFs) catalysts derived from hierarchical M-FeCo-ZIFs-X was prepared. The micropores in M-FeCo-N-C-X have strong capability in O2 capture as well as dictate the nucleation and early-stage deposition of Li2O2,the mesopores provided a channel for the electrolyte wetting, and the macroporous structure promoted more available active sites when used as cathode for Li-O2 batteries. More importantly, M-Fe CoN-C-0.2 based cathode showed a high initial capacity(18,750 mAh g-1@0.1 A g-1), good rate capability(7900 m Ah g-1@0.5 A g-1), and cycle stability up to 192 cycles. Interestingly, the FeCo-N-C-0.2 without macropores suffered relatively poorer stability with only 75 cycles, although its discharge capacity was still as high as 17,200 mA h g-1(@0.1 A g-1). The excellent performance attributed to the synergistic contribution of homogeneous Fe, Co nanoparticles and N co-doping carbon frameworks with special micro–meso-macroporous structure. The results showed that hierarchical FeCo-N-C architectures are promising cathode catalysts for Li-O2 batteries.

关键词： Micro–meso-macroporous FeCo-N-C Li-O2 battery Cathode catalyst Oxygen evolution/reduction reaction

Recent Advances in Non-Precious Metal-Nitrogen-Carbon Single-Site Catalysts for CO_(2)Electroreduction Reaction to CO

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Electrochemical Energy Reviews 2022年第4期5卷 222-252页

作者： Yiqun Chen Junru Zhang Lijun Yang xizhang wang Qiang Wu Zheng Hu Key Laboratory of Mesoscopic Chemistry of MOE School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023JiangsuChina

The carbon dioxide electroreduction reaction(CO_(2)RR)to fuels and/or chemicals is an efficient prospective strategy to realize global carbon management using intermittent electric energy harvested from renewable *** efficient inexpensive electrocatalysts are required to achieve high energy and Faradaic efficiencies as well as fast ***-nitrogen-carbon(M-N-C)single-site catalysts(SSCs)are highly competitive over precious metal catalysts in the CO_(2)RR to CO due to their high performance,easy regulation and low *** the past six years,intensive studies of M-N-C SSCs for CO_(2)RR to CO have been performed,and great progress has been *** review focuses on the important topic of CO_(2)RR to CO with M-N-C *** first introduce the reaction mechanism of the CO_(2)RR to CO and the regulation of the electronic structure from a theoretical ***,the construction of M-N-C SSCs and the regulation of the electronic structure are demonstrated *** up-to-date electrocatalytic performance of M-N-C SSCs with different metal centers(Ni,Fe,Co and others)is summarized and compared systematically to highlight structure-performance correlations that were considered from both theoretical and experimental ***,the opportunities,challenges and future outlooks are summarized to deepen and widen research and applications in this promising field.

关键词： CO_(2)electroreduction reaction Metal-nitrogen-carbon Single-site catalysts Electronic structure CO

Pentacene thin film transistor with low threshold voltage and high mobility by inserting a thin metal phthalocyanines interlayer

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Science China(Technological Sciences) 2012年第2期55卷 417-420页

作者： LI Yi LIU Qi wang xizhang SEKITANI Tsuyoshi SOMEYA Takao HU Zheng Key Laboratory of Mesoscopic Chemistry of MOE School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210093China Department of Applied Physics Tokyo University7-3-1 HongoBunkyo-kuTokyo 113-8656Japan

We herein report the effective performance enhancement of the pentacene-based organic thin film transistors with silicon di- oxide dielectric by inserting a thin metal phthalocyanines interlayer between Au source/drain electrodes and the pentacene active layer. The threshold voltage decreased remarkably from ca. -20 V to a few volts （below -7.6 V） while the mobility in- creased 1.5-3 times after the insertion of the interlayer of only ca. 2 nm, which could be attributed to the reduction of the car- tier injection barrier. The results suggest a simple and effective way to achieve low-threshold-voltage pentacene-based organic thin film transistors with high mobility on silicon dioxide dielectric.

关键词： low threshold voltage and high mobility pentacene-based organic thin film transistors metal phthalocyanines interlayer