超薄双金属氢氧化物纳米片的干法剥离用作氧析出反应电催化剂

<正>体相层状双金属氢氧化物(layered double hydroxides,简称LDHs)由于其独特的二维结构、大的比表面积以及其特殊的电子结构显示出良好的电催化性能,其用于氧析出反应(oxygen evolution reaction,简称OER)已有了广泛的研究~1。但是,大的颗粒尺寸和颗粒的厚度限制了电催化活性位点的暴露从而抑制了其OER的电催化活性。研究表明,相比体相LDHs,单层的二维超薄LDHs纳米片具有更高的比表面,易于暴露更多的电催     

层状双金属氢氧化物基光催化剂的研究进展

层状双金属氢氧化物(LDHs)具有组分可调、层板金属离子高度分散、层间阴离子可交换、拓扑转变等特性,使其可作为理想的光催化剂、催化剂载体或前驱体。作为一种新型多功能材料,LDHs基光催化剂在环境净化、能源储备、工业催化和生物医学等多个领域广泛应用。但是,选择合适的路径进一步优化LDHs基光催化剂的性能,以实现太阳能的高效利用及催化反应过程的高转化率和高选择性仍然具有很大的挑战性。本文依据LDHs的结构特点及活性组分引入方式,将LDHs基光催化剂的制备方法总结归纳为主体层板构筑法、客体插层敏化法、剥离层层组装法、复合材料杂化法四类,详细介绍了不同制备方法对光催化性能的影响,综述其最新研究进展;并结合LDHs基光催化材料的应用,介绍其光催化行为和机理;最后,对LDHs基光催化剂的应用前景进行分析和展望。     

水滑石(LDHs)及其衍生物在生物医药领域的研究进展

生物医学涉及到人类健康相关的多个领域: 临床医疗、公共卫生、医药研发等多个方面. 其中在医药研发领域, 基于插层结构的纳米药物载体的研发已经成为重要发展方向之一. 水滑石(LDHs)及其衍生物具有成本低、合成简单、载药高效、细胞膜透过率高、生物相容性好、易降解等优点, 在生物医药领域得到了广泛关注. 本文主要介绍了LDHs及其衍生物的制备方法, 以及在抗菌治疗、生物成像和肿瘤治疗等方面的应用. 此外, 还简述了LDHs材料的规模化生产方法和现状, 进一步分析了LDHs的实际应用前景. 最后, 对LDHs材料在生物医药领域的未来发展方向进行了展望.     

层状双金属氢氧化物基光催化剂研究进展

层状双金属氢氧化物(LDHs)具有组分可调、层板金属离子高度分散、层间阴离子可交换、拓扑转变等特性,使其可作为理想的光催化剂、催化剂载体或前驱体。作为一种新型多功能材料,LDHs基光催化剂在环境净化、能源储备、工业催化和生物医学等多个领域广泛应用。但是,选择合适的路径进一步优化LDHs基光催化剂的性能,以实现太阳能的高效利用及催化反应过程的高转化率和高选择性仍然具有很大的挑战性。本文依据LDHs的结构特点及活性组分引入方式,将LDHs基光催化剂的制备方法总结归纳为主体层板构筑法、客体插层敏化法、剥离层层组装法、复合材料杂化法四类,详细介绍了不同制备方法对光催化性能的影响,综述其最新研究进展;并结合LDHs基光催化材料的应用,介绍其光催化行为和机理;最后,对LDHs基光催化剂的应用前景进行分析和展望。     

类水滑石材料主客体插层结构的构筑及特性的理论研究

因主体层板和层间客体具有丰富的可调性, 类水滑石材料(LDHs)在催化、 吸附、 生物医药及光、 电、 磁等方面展现出了广阔的应用前景. 近年来理论研究已成为揭示LDHs微观结构和性质的重要手段, 本文系统综述了LDHs材料主体结构、 客体结构以及主客体相互作用3个方面的理论研究工作进展, 及其在作为光驱动催化剂方面应用的理论研究. 从主体元素构成、 元素比例、 电荷分布、 拓扑结构转变、 能带结构、 态密度、 层间阴离子组成、 离子交换性能、 主客体作用力、 能量性质及光催化性能等方面, 在原子、 电子尺度上揭示了LDHs材料结构-性能之间的构效关系, 为以其为材料平台构筑一系列基于超分子插层结构主客体间相互作用的新型功能材料、 扩展材料的功能性提供了丰富的理论信息和有益指导.     

LDHs薄膜基纳米荧光传感器的制备及其研究进展

层状复合氢氧化物(LDHs)是一种层板金属元素和层间离子可调的无机层状材料,利用其独特的插层组装特性,基于静电、氢键、范德华力等相互作用力,功能性荧光客体分子可与LDHs纳米片复合构筑多功能荧光薄膜材料.LDHs薄膜基荧光材料用于荧光传感器,在有机挥发性气体(VOCs)、温度、压力、重要生物分子等的检测中显示了良好性能.本文总结了LDHs复合薄膜的制备方法以及近年来其在纳米荧光传感领域的进展,并对其未来发展做出了展望.     

基于LDHs荧光材料的组装及二维限域效应研究

近年来,层状双金属氢氧化物(LDHs)因其特殊的二维结构及限域环境,作为主体材料构筑了一系列性能优异的插层结构材料,在发光、成像、传感等领域显示了广泛的应用前景.本文从插层客体、组装方法及LDHs的二维限域效应等方面详细介绍了基于LDHs荧光材料的最新研究进展,讨论了二维限域效应与发光性能的内在关联,并探讨了LDHs材料在该领域面临的挑战和发展趋势.     

不同溶剂对甲氨蝶呤/类水滑石复合物性质的影响

采用共沉淀法将甲氨蝶呤(MTX)插层组装到类水滑石(LDHs)层间,分别考察了不同溶剂(如:水、乙醇/水、聚乙二醇-400/水、聚乙二醇-4000/水)对合成的甲氨蝶呤/类水滑石(MTX/LDHs)纳米复合物性质的影响.利用透射电镜(TEM)和原子力显微镜(AFM)观察产物形貌,利用X-射线衍射(XRD)、傅里叶变换红外(FTIR)、热重/差式扫描量热(TG-DSC)和紫外光谱(UV-Vis)等表征手段,对纳米复合物的结构及热力学性质进行了系统的研究.在pH=7.4的磷酸盐缓冲溶液中测定不同时间点药物累积释放量,考察了不同溶剂中合成的MTX/LDHs纳米复合物的药物控释性能.结果表明,短链聚乙二醇的加入保证了纳米粒子的稳定生长,能有效控制产物形貌,合成出的产物呈规则的圆片状,单分散性好,药物缓释性能平稳,释放过程属于药物扩散控制过程.当聚乙二醇分子链过长时,由于其自身容易发生缠绕,反而不利于纳米粒子的生长.     

聚N-异丙基丙烯酰胺/类水滑石复合水凝胶的制备及温敏性

以类水滑石(LDHs)和N-异丙基丙烯酰胺(NIPA)为原材料,采用自由基引发聚合制得了有机无机PNIPA/LDHs温度敏感复合水凝胶。 通过热重分析仪(TGA)、示差扫描量热仪(DSC)和扫描电子显微镜(SEM)等技术手段表征了材料的结构和性能。 结果表明,PNIPA/LDHs复合水凝胶在33 ℃左右可实现溶胶-凝胶的可逆性变化,LDHs质量分数基本不影响复合水凝胶的胶凝化温度和胶凝时间。 LDHs添加可使PNIPA/LDHs复合水凝胶的热稳定性较NIPA有大幅度提升。 随LDHs质量分数及n(Mg):n(Al)的增加,复合凝胶的吸热峰值稍有增加。 所合成PNIPA/LDHs复合水凝胶表面粗糙不平,具有一定的孔洞结构。     

层状复合氢氧化物的有机改性方法及应用研究进展

层状复合氢氧化物(LDHs)因其化学组成可调、比表面积大、生物相容性好等特点,目前在环境、能源和生物医药等领域广受关注.然而, LDHs在合成过程中由于其分子内作用力易发生团聚而导致其在基体中的分散不均匀,极大地限制了LDHs在实际中的应用.有机改性是改善LDHs分散性的有效方法,从表面改性和插层改性两个方面综述了近年来LDHs的有机改性方法,并介绍了其在阻燃、吸附、催化、气体阻隔、发光、储能和生物医药材料等领域的应用.最后对改性后LDHs未来的研究方向和应用领域进行了展望.     

Remote Synthesis of Layered Double Hydroxide Nanosheets Through the Automatic Chemical Robot

As a family of two-dimensional functional materials, layered double hydroxides(LDHs) have the characteristics of adjustable lamellar element type and proportion, variable interlamellar anion, controllable particle size and thickness, providing a robust platform for photo/electro/thermal-catalysis. With the continuous progress of materials science, the synthesis of LDHs is becoming more and more refined. Herein, to achieve the fine preparation of LDHs materials, especailly for the no-chemical/material researchers, we successfully assembled the automatic synthesis device and wrote corresponding computer software to control this device, and the automatic synthesis of bulk and monolayer LDHs nanosheets on a laboratory scale can be realized. This work paves a new labor-saving way for the fine synthesis of LDHs nanostructures, further improving the development of LDHs-based materials.     

Active‐Oxygen‐Enhanced Homogeneous Nucleation of Lithium Metal on Ultrathin Layered Double Hydroxide

The development of safe lithium‐metal anodes is crucial for the next‐generation rechargeable batteries. To stabilize Li metal anodes, pre‐planting Li nucleation seeds on lithiophilic substrates is an efficient strategy to regulate initial nucleation process of Li metal. Now, activated ultrathin layered double hydroxide (U‐LDHs) are reported as a promising lithiophilic 2D material to realize the uniform deposition of Li metal. The experimental studies and DFT calculations reveal that the active oxygen on U‐LDHs provides abundant atomic‐scale active sites for Li homogeneous nucleation and plating. Moreover, the lithiophilic properties of active oxygen is also related to its coordination environments. This work opens up an opportunity to more accurate regulation and understanding of Li nucleation from atomic‐scale based on 2D ultrathin materials.     

Recent progress on preparation and applications of layered double hydroxides

The properties of layered double hydroxides (LDHs), including the adjustability of cations in host layers, exchangeability of anions between layers, and tunability of the crystal structure, render them unique characteristics in preparation and applications. Relating to the structural characteristics of LDHs, this work analyzes the research status, advantages and disadvantages of the synthetic methods for LDHs, including hydrothermal, electrodeposition, co-precipitation and anion exchange methods. In addition, the application status and prospects are reviewed, such as photo/electrocatalysis, electrochemical energy storage, magnetic materials, pollutant adsorption, and other fields. Lastly, the critical issues and solutions in the developing process of LDHs are analyzed and proposed.     

层状材料及催化

LDHs（1ayered double hydroxides）是一类结构可调的阴离子层状及插层结构功能材料,近些年来在催化领域得到了广泛的关注．本文综述了有关LDHs材料构筑原则的理论研究、组装方法及其在多相催化领域应用的最新进展．     

阴离子层状材料的可控制备

LDHs (layered double hydroxides)是一类具有相同结构、不同物理化学性质的阴离子层状无机功能材料,作为催化剂、催化剂载体和催化剂前驱体在催化领域得到了广泛的关注. 本文综述了LDHs制备技术的最新发展,并从粒径控制、结晶度控制、形貌控制、含贵金属LDHs以及原位固载化等方面详细讨论了LDHs的可控制备技术.     

层状复合金属氢氧化物：结构、性质及其应用

本文评述层状复合金属氢氧化物(layered double hydroxides，LDHs)的化学及其应用。层状复合金属氢氧化物具有结合紧密的氢氧化物层和处于层间的阴离子，其比较突出的化学性质是可逆的阴离子交换和热分解性质。不过，因为受到氢氧化物层的局限，处于层间的阴离子表现出的特殊化学性质近年来也越来越受到重视。利用上述三个方面的性质，人们发掘了层状复合金属氢氧化物在材料(包括有机无机复合材料)制备、离子交换与有害阴离子脱除、异构体化学分离、化学反应控制、阻燃材料、活性分子储存与缓释、局部化学反应合成、催化剂及催化剂载体等方面的应用。     

Large continuous, transparent and oriented self-supporting films of layered double hydroxides with tunable chemical composition

Highly ordered transparent self-supporting films of layered double hydroxides (LDHs) with a size of the order of cm2 have been obtained by a simple method; the chemical composition of both the layers and interlayers can be readily tuned, as demonstrated by the preparation of [ZnAl-NO3] LDH, [NiAl-NO3] LDH and [Tb(EDTA)]- intercalated-ZnAl LDH films.     

Single-step synthesis of layered double hydroxides ultrathin nanosheets

A novel single-step approach was developed to prepare large-scale MgAl-LDHs ultrathin nanosheets. The key point of the successful realization was that we employed a high concentration of H(2)O(2). Oxygen molecules, derived from in situ decomposition of H(2)O(2), were speculated to be the decisive factor leading to complete separation of LDHs layers. The ultrathin nanosheets were characterized by XRD, TEM, AFM, FT-IR, and TG-DSC. The results indicated that the thickness of these nanosheets was about 1.44 nm, which was almost in perfect agreement with the theoretical thickness of two LDHs layers. From the TG-DSC curves, the weight loss of these exfoliated MgAl-LDHs ultrathin nanosheets at 500°C was 18.5%, which was much smaller compared to the 32.3% weight loss of unexfoliated MgAl-LDHs.     

Layered Double Hydroxide Nanosheets with Multiple Vacancies Obtained by Dry Exfoliation as Highly Efficient Oxygen Evolution Electrocatalysts

Layered double hydroxides (LDHs) with two-dimensional lamellar structures show excellent electrocatalytic properties. However, the catalytic activity of LDHs needs to be further improved as the large lateral size and thickness of the bulk material limit the number of exposed active sites. However, the development of efficient strategies to exfoliate bulk LDHs into stable monolayer LDH nanosheets with more exposed active sites is very challenging. On the other hand, the intrinsic activity of monolayer LDH nanosheets can be tuned by surface engineering. Herein, we have exfoliated bulk CoFe LDHs into ultrathin LDH nanosheets through Ar plasma etching, which also resulted in the formation of multiple vacancies (including O, Co, and Fe vacancies) in the ultrathin 2D nanosheets. Owing to their ultrathin 2D structure, the LDH nanosheets expose a greater number of active sites, and the multiple vacancies significantly improve the intrinsic activity in the oxygen evolution reaction (OER).     

Heterogeneous ultrathin films fabricated by alternate assembly of exfoliated layered double hydroxides and polyanion

Transparent heterogeneous ultrathin films of exfoliated layered double hydroxide (LDHs) nanosheets, fabricated alternately with polyanion, have been obtained via a layer-by-layer electrostatic self-assembly which yields a series of novel LDH films with potential multifunctionality.