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| 1 | Fe_3O_4/g-C_3N_4复合催化剂增强芬顿/光-芬顿和类过氧化酶反应的活性及稳定性(英文)显示文摘石墨相的氮化碳(g-C_3N_4)已被广泛用于光催化、水分解、光子检测器、电池、以及光电阴极.与其他光催化材料相比,g-C_3N_4具有价格低廉,易制备,无毒无污染等优点.此外,C_3N_4具有适宜的带隙(2.7 eV),能有效地吸收可见光.有关C_3N_4的光催化研究很多,但是其降解效率受限于电子空穴对的快速复合.因此,为了提高C_3N_4光催化反应效率,需要对其进行改性.磁铁矿(Fe_3O_4)广泛用于光催化和芬顿/光-芬顿反应.Fe_3O_4晶体具有反式尖晶石结构,其中Fe^(2+)和Fe^(3+)同时存在.研究表明,磁铁矿在酸性条件下催化效果显著,然而,它的比表面积小,随着反应时间的推移,铁离子会溶出,不利于有机物降解反应.因此,近来许多研究着重于磁铁矿复合物的制备,以提高磁铁矿的稳定性及催化性能.本文通过惰性氛围高温焙烧三聚氰胺制备了g-C_3N_4,再通过氯化铁和乙酸钠在乙醇中于180°C溶剂热反应,制备Fe_3O_4纳米粒子,最后通过静电自组装过程制备出Fe_3O_4/g-C_3N_4纳米复合材料.利用X射线衍射(XRD),扫描电子显微镜(SEM)及X射线光电子光谱(XPS)等手段验证其组成和结构.XRD结果表明,Fe_3O_4/g-C_3N_4复合材料中可以清晰看到Fe_3O_4和g-C_3N_4的衍射峰,说明这两种材料的晶相得以保持.SEM和TEM结果表明,Fe_3O_4纳米颗粒很好地附着在g-C_3N_4薄片上.XPS结果表明,氮化碳中存在典型的三种N峰;此外还存在铁的两种价态.光-芬顿活性测试中,相同条件下,Fe_3O_4/g-C_3N_4在60 min内将罗丹明B(RhB)几乎降解完全,而单组份的Fe_3O_4或g-C_3N_4对RhB的降解小于50%.可见,复合后的Fe_3O_4/g-C_3N_4光催化性能得到很大提升.单g-C_3N_4本身由于快速的电子空穴复合以及对双氧水的弱亲和力,因而对Rh B降解效果差.单独的Fe_3O_4由于在中性或者碱性条件下反而会抑制光催化芬顿活性.对于制备的Fe_3O_4/g-C_3N_4复合材料,具有以下优点:(1)电子在Fe^(3+)和g-C_3N_4的LUMO轨道上的转移降低了电子-空穴对的复合;(2)Fe_3O_4均匀分布在g-C_3N_4上,对于H_2O_2的吸附提供了有利的高比表面积;(3)Fe_3O_4和g-C_3N_4之间的界面相互作用使得Fe_3O_4的稳定性提高.通过降解RhB的动力学研究,得到反应速率为0.02 min^(–1),属准一级反应.分析检测结果表明,光-芬顿反应后,RhB分子被彻底矿化降解,没有中间产物生成,最终降解为CO_2和水.同时,通过对辣根过氧化物酶(HRP)模拟催化进行测试,以3,3',5,5'-四甲基联苯胺盐酸盐(TMB)作为基质,同时添加双氧水和Fe_3O_4/g-C_3N_4,在pH值为4.5条件下,TMB可以被有效氧化.实验表明,Fe_3O_4/g-C_3N_4添加量为25 mg/ml时,对TMB氧化性能最佳.复合催化剂还用于多巴胺的催化氧化反应.结果表明,多巴胺的氧化反应速率常数为1.21 min^(–1),属一级动力学反应.总之,复合材料提高了Rh B的光催化降解活性和稳定性;对TMB和HRP亲和性好,表现出高的类过氧化酶反应活性;有效的多巴胺氧化反应表明其有望用于生物基氧化反应中.实验结果表明,本文发展的Fe_3O_4/g-C_3N_4复合材料为其他类型复合材料的制备与应用提供了新的思路. | Shafaq Sahar Akif Zeb 刘亚男 Naseeb Ullah 徐安武 | 2017 | Chinese Journal of Catalysis2017,38,12: | 8 |
| 2 | Recent progress in Co-based metal-organic framework derivatives for advanced batteries显示文摘To date,Co-based metal-organic frameworks(Co-MOFs)have drawn much attention owing to their advantages of easy preparation,high porosity and adjustable structure.Because of these enticing properties,numerous efforts have been devoted to their applications in energy storage and conversion.However,poor conductivity has become one of the biggest obstacles for large-scale use of pristine Co-MOFs.Subsequently,many attempts have been carried out to develop various Co-MOF derived materials as electrodes for rechargeable batteries in order to address the above-mentioned shortcoming and to enhance the electrical conductivity with improved stability during cycling.Moreover,in addition to improvement of Li-ion batteries in practical utilization,seeking for other rechargeable batteries is another urgent task due to the high cost and limited sources of metallic Li.Herein,by following the recent research progress,this review provides an overview of applications of Co-MOF derived materials in various rechargeable batteries including lithium-ion batteries,sodium-ion batteries,lithium-sulfur batteries,zinc air batteries and other rechargeable batteries,where they have been utilized as cathodes,anodes,separators and electrocatalysts.Accordingly,we categorize and compare the morphology driven electrochemical performance of various Co-MOF derivatives including porous carbon,cobalt oxides,cobalt chalcogenides,cobalt phosphides and corresponding composites.Finally,current challenges for large-scale production and commercialization of Co-MOF derived materials as well as some reasonable solutions have been discussed at the end. | Jianen Zhou Qingyun Yang Qiongyi Xie Hong Ou Xiaoming Lin Akif Zeb Lei Hu Yongbo Wu Guozheng Ma | 2022 | Journal of Materials Science & Technology2022,,1: | 2 |
| 3 | Metal–Organic Frameworks and Their Derivatives as Cathodes for Lithium‑Ion Battery Applications:A Review显示文摘The development of energy storage technology is important for resolving the issues and challenges of utilizing sustainable green energy in modern-day society.As an emerging technology,lithium-ion batteries(LIBs)are a common source of power for a wide variety of electronic devices,and major advances require the development and exploitation of new electrode materials;thus,fundamental knowledge of their atomic and nanoscale properties is necessary.By moving beyond conven-tional cathode candidates,metal–organic frameworks(MOFs)chemistry provides an excellent direction for designing and developing promising high-performance cathode materials for use in LIBs.Here,we carry out an overarching discussion on the development and application of MOFs and their derivatives as cathodes for lithium-ion battery applications.A timely overview of the exciting progress of MOFs as well as MOF-derived metallic components is highlighted.The unique char-acteristics of MOFs,such as their large surface area,high tunable porosity with uniform pore size,unique structural and morphological features,controllable framework composition and low densities,combine together to provide good interfacial charge transport properties and short diffusion lengths for electrons and/or ions that adequately support electrochemical redox reactions.The progress of MOFs and their derived composites as cathode candidates for LIBs is emphasized based on their electrochemical results,while also discussing the remaining issues and potential upcoming research directions. | R.Chenna Krishna Reddy Xiaoming Lin Akif Zeb Cheng‑Yong Su | 2022 | Electrochemical Energy Reviews2022,5,2: | 1 |
| 4 | Carbon‐encapsulated anionic‐defective MnO/Ni open microcages: A hierarchical stress‐release engineering for superior lithium storage显示文摘Rational manipulation of multicomponent materials into a sophisticated architecture is a prerequisite for developing lithium‐ion batteries.However,mechanical diffusion‐induced strain accumulation leads to sluggish diffusion kinetics and anomalous structure instability,further resulting in inferior long‐term cyclability and rate performance.Herein,the von Mises stress distribution on open microcages composed of secondary nanoparticles(OCNs)is mechanically investigated by finite element simulation,which elucidates the pronounced stress‐release effect on OCNs architecture.Afterward,a facile metal–organic framework‐derived methodology is proposed for constructing multihierarchical carbon‐encapsulated oxygen vacancy‐enriched MnO/Ni OCNs(OV‐MnO/Ni OCNs).Due to structural and compositional integration,the OV‐MnO/Ni OCNs achieve extraordinary lithium storage performance with excellent reversible capacity(1905.1 mAh g^(−1) at 0.2 A g^(−1)),ultrahigh cycling stability(1653.5 mAh g^(−1) at 2 A g^(−1) up to 600 cycles),and considerable rate capability(463.3 mAh g^(−1) even at 10 A g^(−1)).The primary lithium storage mechanisms are further systematically determined by experimental and theoretical investigations.The enriched oxygen vacancies,metallic Ni configuration,and N‐doped carbonaceous matrix provide more active sites,construct omnidirectional diffusion pathways,suppress volume expansion,and boost electronic conductivity,thus yielding an exceptional diffusivity coefficient and expedited electrochemical kinetics.This study offers profound insights for the elaborate design of multicompositional electrodes into a mechanical stress‐release structure toward advanced energy storage application and development. | Jia Lin Yingying Peng Reddivari Chenna Krishna Reddy Akif Zeb Xiaoming Lin Yan-Hui Sun | 2023 | Carbon Energy2023,5,1: | 1 |
| 5 | Molecular and atomic manipulation of metal-organic framework-derived LiCoMnO_(4):An oxygen-deficient strategy for advanced lithium storage显示文摘As a novel class of high-voltage cathode materials,spinel lithium transition metal oxides have been faced with demerits including pronounced structural instability caused by Jahn-Teller distortion(especially at the lower voltage region)and severe capacity degradation despite their intriguing electrochemical properties.To extend their functionalities as broad-voltage cathodes,the sacrificial template method has been regarded as a promising way to realize structural and compositional control for desirable electrochemical behaviors.Herein,we report a synthetic protocol to directionally prepare Li Co Mn O_(4)(LCMO)using carboxyl-based metal-organic frameworks(MOFs)as self-sacrificing templates.Impressively,LCMO derived from Co Mn-BDC(H_(2)BDC=1,4-benzenedicarboxylate)displays superior electrochemical performances with a specific capacity of 151.6 m Ah g^(-1)at 1 C(150 m A g^(-1))after 120 cycles and excellent rate capacity of 91.9 m Ah g^(-1)at 10 C due to the morphology control,microstructural modulation,and atomic manipulation of the MOF precursor.Bestowed by the optimized atomic and electronic structure,abundant oxygen vacancies,and the nanostructure retained from MOF precursors,LCMO materials display extraordinary electrochemical properties,which have been extensively verified by both experimental and theoretical studies.This work not only provides guidelines for the directional design of spinel materials at molecular and atomic levels but also sheds light on the practical use of LIBs with broad range voltage. | Jian-En Zhou Jiahao Chen Xiaoke Zhang Akif Zeb Xiaoming Lin | 2022 | Journal of Energy Chemistry2022,,12: | 0 |