Carbon-doped CuFe_(2)O_(4) with C-O-M channels for enhanced Fenton-like degradation of tetracycline hydrochloride: From construction to mechanism

Carbon-doped copper ferrite(C–CuFe_(2)O_(4))was synthesized by a simple two-step hydrothermal method,which showed enhanced tetracycline hydrochloride(TCH)removal efficiency as compared to the pure CuFe_(2)O_(4) in Fenton-like reaction.A removal efficiency of 94%was achieved with 0.2 g L^(-1) catalyst and 20 mmol L^(-1) H_(2)O_(2) within 90 min.We demonstrated that 5%C–CuFe_(2)O_(4) catalyst in the presence of H_(2)O_(2) was significantly efficient for TCH degradation under the near-neutral pH(5–9)without buffer.Multiple techniques,including SEM,TEM,XRD,FTIR,Raman,XPS M€ossbauer and so on,were conducted to investigate the structures,morphologies and electronic properties of as-prepared samples.The introduction of carbon can effectively accelerate electron transfer by cooperating with Cu and Fe to activate H_(2)O_(2) to generate·OH and·O_(2)^(-).Particularly,theoretical calculations display that the p,p,d orbital hybridization of C,O,Cu and Fe can form C–O–Cu and C–O–Fe bonds,and the electrons on carbon can transfer to metal Cu and Fe along the C–O–Fe and C–O–Cu channels,thus forming electron-rich reactive centers around Fe and Cu.This work provides lightful reference for the modification of spinel ferrites in Fenton-like application.

Plasmonic Ag nanoparticles decorated MIL-101(Fe) for enhanced photocatalytic degradation of bisphenol A with peroxymonosulfate under visible-light irradiation

Photocatalytic activation of peroxymonosulfate (PMS) has garnered a lot of interest in the field of wastewater treatment. Herein, a plasmonic Ag nanoparticles decorated MIL-101(Fe) hybrid was synthesized through a photodeposition process. Upon light irradiation, the Ag/MIL-101(Fe) exhibit reinforced photocatalytic activities for elimination of bisphenol A (BPA) with PMS. The optimized 2.0% Ag/MIL-101(Fe) composite presented the highest photocatalytic activity with kinetic constant k of 0.102 min-1, which was about 10-fold of the pristine MIL-101(Fe). Loading of plasmonic Ag into MIL-101(Fe) boosts photoinduced carrier separation and accelerates PMS activation to generate strong oxidative radicals. Photoelectrochemical tests and multiple spectroscopic studies confirmed the promoted charge carrier separation and transfer capability of Ag/MIL-101(Fe). Combining the results of radical trapping experiments and electron spin resonance (ESR), the formed SO4·-, ·OH, ·O2- and 1O2 had a significant role in the photocatalytic process. According to intermediate study, the degradation pathway was studied, and the possible mechanism was proposed.

Boost VS_(2) electrochemical reactive kinetics by regulating crystallographic planes and coupling carbon matrix for high performance sodium-ion storage

Vanadium disulfide(VS_(2)) as a typical two-dimensional transition metal chalcogenide has excellent competitiveness for sodium-ion storage due to its wide layer spacing(0.575 nm),high theoretical capacity of 932mAh·g^(-1) originating from multi-electron electrochemical redox.However,continuous sodiation process accompanied by crystal structural evolution and collapse cause rapid capacity decaying.Herein,novel few-layer VS_(2)nanosheets with open(001) crystal planes are in-situ constructed on reduced graphene oxide to solve these issues mentioned above.It indicates that few-layer VS_(2)provides more Na^(+) storage activity due to the low Na^(+)surface migration energy barrier on exposed crystal(001)planes.The flexible and high electronic conductivity of carbon matrix also effectively builds multi-level buffer structure and electron transport kinetics to boost the Na^(+)insertion/conversion reactive activity on VS_(2) as well as Na^(+) pseudocapacitance storage kinetics on edges and defects of nano sheets.Those coupling effects result in high rate capability and long cycling stability as a battery/capacitor anode.It delivers conspicuous high energy density of 81 and 40 Wh·kg^(-1) at power density of 118 and 10,286W·kg^(-1),as well as 80% energy retention rate after 5000cycles,confirming its great application potential in sodiumbased storage devices.

高电容性能MXene电极对插层修饰离子的选择性

离子插层是提高Ti_(3)C_(2)TxMXene电化学性能的有效方法之一.然而,不同的插层离子对MXene的结构和电化学性能的影响是否相同这一问题尚不清楚.本文系统研究了Li+、Na+、K+、Cs+、Zn2+、Mg2+、SO_(4)2-和OH-等一系列离子插层后的MXene的结构特征和电化学性能.研究结果表明,插层离子的半径、电荷数和化学特性对插层效果都会产生影响.在所研究的插层剂中,由离子半径最大的一价阳离子Cs+和具有强碱性的阴离子OH-组成的插层剂CsOH对MXene具有较好的插层效果.插层后的MXene层间距增大,层间容纳了大量游离水,Ti的价态升高,片层表面有利于氧化还原反应的含O官能团增多,这都大大促进了电解液离子H+的扩散与存储.由此制备的电极的质量比电容大幅度提高,为原始MXene电极的7倍多,而且经过20,000次充放电循环后电容保持率未发生下降.本文为具有高电容性能的MXene和MXene基复合电极的合理设计和制备提供了指导.

rGO空间限域生长超薄In_(2)S_(3)纳米片用于构建高效准一维Sb_(2)Se_(3)基异质结光阴极

硒化锑(Sb_(2)Se_(3))属于窄带隙半导体材料,具有良好的光吸收特性,已逐渐应用于光电催化领域.独特的一维(Sb_(4)Se_(6))_(n)带状结构单元连接方式,使其载流子传输具有高度各向异性.本文通过气相输运沉积法和原位水热法成功构建了还原氧化石墨烯(rGO)修饰的准一维Sb_(2)Se_(3)@In_(2)S_(3)光陷阱异质结.研究结果表明,在rGO空间限域效应下,原位生长的非层状In_(2)S_(3)纳米片厚度从30 nm减小到10 nm,显著增加了光电极的电化学活性比表面积,进一步增强了光陷阱纳米结构对光的捕获能力.rGO和超薄In_(2)S_(3)纳米片共同修饰的准一维毛刷状Sb_(2)Se_(3)@In_(2)S_(3)-rGO纳米棒光电极在0 V(相对于可逆氢电极)的外加偏压下,光电流密度可达1.169 m A cm^(-2),约是Sb_(2)Se_(3)@In_(2)S_(3)和单体Sb_(2)Se_(3)的2倍和16倍,且稳定性良好,在中性条件下平均产氢速率为16.59μmol cm^(-2)h^(-1).实验结果和理论计算均表明,Ⅱ型异质结电荷传输方式是其光电化学增强的物理机制.以上工作为设计基于rGO修饰的复合光电极用于光电化学领域的研究提供了崭新的思路.

Heterostructured NiS_(2)@SnS_(2) hollow spheres as superior high-rate and durable anodes for sodium-ion batteries

Tin-based sulfides have attracted increasing attention as anodes for sodium-ion batteries(SIBs) owing to their high theoretical capacity;however, the poor rate capability and inferior cycling stability caused by the low electrical conductivity, sluggish kinetics and drastic volume variations during cycling have greatly hampered their practical applications. Herein, heterostructured NiS_(2)@SnS_(2) hybrid spheres were delicately designed and constructed by anchoring interconnected SnS_(2) nanosheets on metalorganic frameworks(MOFs)-derived Ni S_(2) hollow spheres coupled with N-doped carbon skeleton through facile solvothermal and sulfurization/carbonization processes. The unique hollow heterostructure with highly conductive carbon matrix can effectively facilitate the charge transfer kinetics and ensure the desired buffer space while endowing more active sites and enhanced structural integrity, as demonstrated by the experimental and density functional theory(DFT) results. Benefitting from these merits, the NiS_(2)@SnS_(2) hybrid composite displays a high reversible capacity of 820 m Ah g^(-1) after 250 cycles at 1 A g^(-1), and retains a value of 673 m Ah g^(-1)after 1,300 cycles at 5 A g^(-1), manifesting the excellent high-rate and durable sodium storage behaviors when applied in SIBs. This study shall shed more light on the fabricating and interface engineering of other transition metal-based composite anodes for high-performance SIBs.

基于受体修饰的双层有机场效应晶体管化学传感器用于高灵敏检测锂离子电池电解液泄漏

易燃易爆的锂离子电池电解液泄漏是电池故障的早期症状之一,甚至会导致电池自燃或电动汽车爆炸.因此,有必要找到一种快速简单的方法来监测电解液泄漏.现有的传感器难以有效且快速地检测微量电解液泄漏.我们首次提出了一种将有机场效应晶体管(OFET)的灵敏度和联二脲受体的选择性相结合,以检测电池电解液泄漏的策略.复合后的传感器与没有受体的原始传感器相比,灵敏度显著提高,传感器对碳酸二乙酯的检测限低至1.4 ppm.并且可以在几秒钟内有效地检测到微量的泄漏, 200 n L电解液泄漏能够导致3%的响应.受体复合后的OFET传感器的优异性能使其成为锂离子电池安全监测的良好候选者,并为传感技术的发展提供了一个有前途的平台.

Regulating nitrogen vacancies within graphitic carbon nitride to boost photocatalytic hydrogen peroxide production

Introducing nitrogen vacancies is an effective method to improve the catalytic performance of g-C_(3)N_(4)-based photocatalysts,whereas understanding how nitrogen vacancies types affect the catalytic performance remains unclear.Herein,two different types of nitrogen vacancies were successfully introduced into g-C_(3)N_(4)by pyrolysis of melamine under argon and ammonia atmosphere with subsequent HNO3 oxidation.The pyrolysis atmosphere is found to have a significant influence on the introduced nitrogen vacancies type,where tertiary nitrogen groups(N_(3)C)and sp2-hybridized nitrogen atoms(N_(2)C)were the preferred sites for the formation of nitrogen vacancies under ammonia and argon pyrolysis,respectively.Moreover,nitrogen vacancies from N3C are experimentally and theoretically demonstrated to facilitate the narrowed band gap and the improved oxygen absorption capability.As expected,the optimal catalyst exhibits high H_(2)O_(2)yield of 451.8µM,which is 3.8 times higher than the pristine g-C_(3)N_(4)(119.0µM)after 4 h and good stability after10 photocatalytic runs.