基于Ti3C2-MXene的太阳能界面水汽转换

水资源匮乏是现代化发展中面临的全球性问题,太阳能界面水汽转换(Interfacial Solar Steam Generation,ISSG)是一种高效、绿色、低成本进行海水淡化和废水处理的方法.ISSG使用绿色的太阳能作为热源,通过光热转换并将热限制在水气界面上以高效产生蒸气,然后经过冷凝收集获得清洁水.设计和构筑具...     

ZIF-8衍生的具有可控氧空位的ZnO对光催化去除NO的增强及毒性NO2形成的抑制

氧化锌作为一种半导体材料,具有合适的能带结构位置,高催化效率,低成本和环境可持续性,因而广泛用于光催化领域.然而,由于氧化锌的宽带隙,可见光吸收能力差以及光生电子-空穴对的快速复合,极大地影响了其光催化效率.通过引入氧空位调控光催化剂的结构被证明是一种可以改善光生载流子的分离,从而提高光催化性能的有效方法.本文以ZIF-8为前驱体,采用两步煅烧法合成了具有不同浓度氧空位分布的ZnO纳米光催化剂,通过X射线衍射(XRD)、扫描电镜(SEM)、透射电镜(TEM)、紫外-可见漫反射光谱(UV-Vis DRS)、X射线光电子能谱(XPS)、电子顺磁共振(EPR)、荧光光谱仪(PL)等手段系统地分析了合成的光催化剂的理化性质,并评价了它们在可见光下光催化氧化去除NO反应性能.EPR结果表明,样品中氧空位的浓度取决于温度处理的过程.通过两步煅烧法得到氧化锌中氧空位的含量高于一步直接煅烧法所得的样品.此外,随着煅烧温度升高,合成的氧化锌晶格越完好,其氧空位含量越少.UV-Vis DRS结果表明,两步煅烧法合成的ZnO与商业的ZnO及一步法直接煅烧合成的ZnO相比,其吸光范围从紫外光拓展到了可见光,表现出了更加优异的吸光性能.光催化反应结果表明,与商业氧化锌和一步直接煅烧法所得样品相比,两步煅烧法合成的样品表现出了更优异的光催化去除NO性能,并抑制了中间产物毒性NO2的产生,促进了NO的深度氧化.具体反应路径为:在光照过程中,光生电子很容易被氧空位俘获,与O2反应产生更多的超氧自由基(·O2^-),从而将NO氧化成最终的产物硝酸盐.尤其有趣的是,先在350 ℃煅烧2小时再400℃煅烧1小时的两步法样品Z 350-400的NO去除效率分别比一步法样品Z 400(400℃煅烧)和商用ZnO高出1.5和4.6倍.这表明以MOF材料衍生的具有适当量氧空位的金属氧化物为一种高效去除NO的光催化剂具有很好的应用前景.     

钼酸根阴离子在增强聚苯胺包覆的镍钴层状氢氧化物的电容和析氧行为中的关键作用

理论容量大且过电位低的层状氢氧化物(LDHs)是极有前景的超级电容电池和析氧反应的电极材料;然而,体相LDHs的低电导率和活性位点不足增加了电极的内阻,降低了电极容量和产氧效率.本文采用两步法制备了聚苯胺包覆的MoO42?插层的镍钴层状双金属氢氧化物复合电极(M-LDH@PANI).随着LDH中MoO42?含量的增加,针状的LDH微球逐渐演化为具有较高比表面积的片状M-LDH微球,这为整个电极提供了更多的电化学位点.此外,非晶态的聚苯胺包覆提高了复合电极的电导率.在引入适量MoO42?插层离子时,M-LDH@PANI表现出显著强化的储能和催化性能.所获得的M-LDH@PANI-0.5在析氧反应中表现出优越的电催化活性(10 mA cm?2时的过电位为266 mV),作为超级电容电池电极则具有864.8 C g?1的高容量.采用M-LDH@PANI-0.5作为正极及以活性炭作为负极组装的超级电容电池在功率密度为8,300.0 W kg?1时能量密度为44.6 Wh kg?1,且具有优异的循环稳定性(10000次循环后保留83.9％的初始容量).本文为LDH基材料的阴离子插层改性增强材料性能的机理提供了一个非传统的解释.在上述研究基础上,采用射线衍射(XRD)、X射线光电子能谱(XPS)、扫描电子显微镜(SEM)、高分辨透射电镜(HRTEM)和比表面积测试(BET)等手段对样品进行了深入表征.XRD结果表明,MoO42?插层的LDH材料的层间晶面(003)的峰随着MoO42?含量的增加而逐渐消失,这是由于晶面间距越大越容易受到晶粒细化的影响,间距大的晶格更容易受到破坏,导致晶格的展宽和弱化,从而间接证明MoO42?的成功插层.SEM、HRTEM和BET测试结果表明,MoO42?的含量对材料的形貌和比表面积具有重大影响.利用XPS对样品的价态进行了研究,发现随着MoO42?含量的增加,Co和Ni的价态没有明显变化.电化学测试结果表明,电极的储能和催化性能随MoO42?含量的增加而先增加后减小.利用理论计算分析了MoO42?在LDH中的插层行为,发现少量的MoO42?有利于扩大LDH的层间间距,而过量的MoO42?则会与LDH的H原子结合,从而与电解液中的OH?竞争,导致复合电极的电化学性能下降.此外,MoO42?插层的片状微球能有效调节材料的去质子化能,大大加速电极表面的氧化还原反应.因此,MoO42?插层能够显著强化LDH基材料的超级电容电池电极和OER催化剂电化学性能.     

压缩CO2中Co-N-C催化3-硝基苯乙烯选择性加氢反应动力学及相行为

对于苯环上含有各种可还原基团(如–C=C,–CN,–C≡C)的硝基芳烃,通过选择性加氢来制备芳香胺类化合物依然充满挑战.负载型纳米催化剂通常存在过度加氢的缺陷,虽然通过覆盖部分金属位点等方法可改善其选择性,但多是以牺牲催化活性为代价.得益于较高的原子利用率以及孤立的活性位结构,单原子催化剂在硝基芳烃选择性加氢反应中崭露...     

基于吡嗪空穴传输层的合成及在p-i-n型钙钛矿太阳能电池中的应用

钙钛矿太阳能电池由于具有高的光电转换效率,简单的溶液加工工艺,较低的成本等优势因而拥有广阔的应用前景。有机小分子空穴传输层材料在钙钛矿太阳能电池中扮演着极其重要的角色。在本工作中,我们设计和合成了基于吡嗪为分子中心核,三苯胺为分枝的X型空穴传输层材料PT-TPA。与Si-OMeTPA对比,吡嗪的引入不仅不会影响其结晶性,并且能够改善其电荷转移特性和分子中心共平面性,从而显著提升了PT-TPA的空穴迁移率。在非掺杂的情况之下,基于PT-TPA空穴传输层的p-i-n型钙钛矿太阳能电池展现出17.52%的光电转换效率,与相同条件下基于Si-OMeTPA空穴传输层的器件相比,效率提高了近15%。     

疏水性低共熔溶剂液液微萃取/高效液相色谱法测定豆奶中三嗪类和苯脲类除草剂

该文建立了一种简单、高效的新型疏水性低共熔溶剂液液微萃取法,用于提取和富集市售包装豆奶中的三嗪类（阿特拉津、去草净）和苯脲类（灭草隆、绿麦隆）除草剂,并结合高效液相色谱对目标分析物进行分离和测定。以六氟异丙醇为氢键供体,四丁基氯化铵为氢键受体,按照不同摩尔比制备了一系列疏水性低共熔溶剂,并对影响萃取效果的实验条件进行了优化,包括低共熔溶剂的种类及用量、氯化钠用量、涡旋时间、pH值和温度。结果表明,在最佳实验条件下,4种目标物在1.00～500.00 μg/L范围内具有良好的线性关系（r ≥ 0.998 4）,检出限和定量下限分别为0.56～0.95 μg/L和1.87～3.16 μg/L,日内和日间相对标准偏差（RSD）分别为0.28%～2.0%和2.1%～7.5%,加标回收率为86.4%～117%。该方法具有操作简单快速、萃取时间短、试剂用量少和实验成本低等优点,可用于市售包装豆奶中三嗪类和苯脲类除草剂的分析检测。     

荧光探针在氰化物分析中的研究进展

氰化物极易与细胞色素氧化酶键合,抑制电子转移、导致组织缺氧,从而显示较强的毒性。荧光化学传感器作为简易、灵敏且可视化的方法广泛应用于氰化物的检测。本文对荧光探针在氰化物检测中的应用进行综述,概述了氰化物的毒性机制和荧光探针对氰化物的响应机理。同时,本文总结了荧光探针在水体、食品和生物组织中对氰化物的检测及生物成像中的应用,并对荧光探针在结构设计中如何提高生物兼容性和靶向性等进行了展望,以期为光化学探针分子的设计及应用提供理论与研究依据。     

Rapid and label-free classification of pathogens based on light scattering,reduced power spectral features and support vector machine

The rapid identification of pathogens is crucial in controlling the food quality and safety. The proposed system for the rapid and label-free identification of pathogens is based on the principle of laser scattering from the bacterial microbes. The clinical prototype consists of three parts: the laser beam, photodetectors, and the data acquisition system. The bacterial testing sample was mixed with 10 mL distilled water and placed inside the machine chamber. When the bacterial microbes pass by the laser beam, the scattering of light occurs due to variation in size, shape, and morphology. Due to this reason, different types of pathogens show their unique light scattering patterns. The photo-detectors were arranged at the surroundings of the sample at different angles to collect the scattered light. The photodetectors convert the scattered light intensity into a voltage waveform. The waveform features were acquired by using the power spectral characteristics, and the dimensionality of extracted features was reduced by applying minimal-redundancy-maximal-relevance criterion (mRMR). A support vector machine (SVM) classifier was developed by training the selected power spectral features for the classification of three different bacterial microbes. The resulting average identification accuracies of E. faecalis,E. coli and S. aureus were 99%, 87%, and 94%, respectively. The overall experimental results yield a higher accuracy of 93.6%, indicating that the proposed device has the potential for label-free identification of pathogens with simplicity, rapidity, and cost-effectiveness.     

Recent advances in the improvement of g-C3N4 based photocatalytic materials

g-C₃N₄ have been widely used in the fields of photocatalytic hydrogen production,photocatalytic degradation of dyes and oxidative degradation of toxic gases due to their excellent performance.It has attracted extensive attention in recent years due to its highly efficient photocatalytic capacity of hydrogen generation,water oxidation,carbon dioxide reduction and degradation of organic pollutants.Because of the abundant carbon and nitrogen composition of the earth,large-scale production and industrial applications of this material are possible.The modification of this material makes its performance more excellent so that this new material can obtain a steady stream of vitality.These outstanding works have become important materials and milestones on the road to mankind's photocatalytic hydrogen production.This review will begin with the basic idea of designing,synthesizing and improving g-C₃N₄ based photocatalytic materials,and introduce the latest development of g-C₃N₄ photocatalysts in hydrogen production from four aspects of controlling the carbon/nitrogen ratio,morphology,element doping and heterojunction structure of g-C₃N₄ materials.     

Comprehensive Mechanism for CO Electroreduction on Dual-Atom-Catalyst-Anchored N-Doped Graphene

Carbon neutrality has drawn increasing attention for realizing the carbon cyclization and reducing the greenhouse effect. Although the C1 products, such as CO, can be achieved with a high Faraday efficiency, the targeted production of C2 fuels as well as the mechanism have not been systematically investigated. In this work, we carry out a first-principles study to screen dual-atom catalysts (DACs) for producing C2 fuels through the electrocatalytic carbon monoxide reduction reaction (e-CORR). We find that methanol, ethanol and ethylene can be produced on both DAC−Co and DAC−Cu, while acetate can be achieved on DAC−Cu only. Importantly, methanol and ethylene are preferred on DAC−Co, while acetate and ethylene on DAC−Cu. Furthermore, we show that the explicit solvent can enhance the adsorption and influence the protonation steps, which subsequently affects the protonation and dimerization behavior as well as the performance and selectivity of e-CORR on DACs. We further demonstrate that the C−C coupling is easy to be formed and stabilized if the Integrated Crystal Orbital Hamilton Population (ICOHP) is low because of the low energy barrier. Our findings provide not only guidance on the design of novel catalysts for e-CORR, but an insightful understanding on the reduction mechanism.