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1Weakly hydrophobic nanoconfinement by graphene aerogels greatly enhances the reactivity and ambient stability of reactivity of MIL-101-Fe in Fenton-like reaction显示文摘In the pursuit of heterogeneous catalysts with high reactivity,metal organic framework(MOF)nanomaterials have received tremendous attentions.However,many MOF catalysts especially Fe-based MOFs need to be utilized immediately after synthesis or being activated using high temperature,because of the easy loss of reactivity in humid environments resulting from the occupation of active Fe sites by water molecules.Here,we describe an inspiring strategy of growing MIL-101-Fe nanoparticles inside the three-dimensional confined space of graphene aerogel(GA),generating shapeable GA/MIL-101-Fe nanocomposite convenient for practical use.Compared to MIL-101-Fe,GA/MIL-101-Fe as catalyst demonstrates much higher reactivity in Fenton-like reaction,attributing to smaller MIL-101-Fe particle size,presence of active Fe(II)sites,and abundant defects in GA.Strikingly,the weakly hydrophobic nature of the composite greatly inhibits the loss of catalytic reactivity after being stored in humid air and accelerates the recovery of reactivity in mild temperature,by resisting the entrance of water molecules and helping to exclude water molecules.This work demonstrates that a delicate design of nanocomposite structure could not only improve the reactivity of the catalytic component,but also overcome its intrinsic drawback by taking advantage of the properties of host.We hope this functional nanoconfinement strategy could be extended to more scenarios in other fields.Yuwei Zhang Fei Liu Zhichao Yang Jieshu Qian Bingcai Pan 2021Nano Research2021,14,7:2
2Rapid and Scalable Synthesis of Prussian Blue Analogue Nanocubes for Electrocatalytic Water Oxidation显示文摘Design and fabrication of earth-abundant electrocatalysts for oxygen evolution reaction(OER)is essential in improving the overall ef-ficiency of water electrolysis.In this work,we proposed a rapid and scalable synthesis route for fabricating Prussian blue analogue(PBA)nano cubes with tun able compositi ons and uniform particle size.With the structural ben efits of abu ndant surface sites,facile charge transfer behavior and favorable Co^(2+)-to-Co^(3+)pre-oxidation reaction,fast generation and accumulation of the catalytically active Co3+sites can be achieved for the CoCo PBA nano cubes,leadi ng to remarkable OER activity with simulta neously achieved low overpotential,large anodic current density,small Tafel slope as well as outstanding intrinsic activity.Of note,by performing Iong-term OER operati on,the CoCo PBA nano cubes exhibit a remarkable 5.5-folds performs nee enhan ceme nt,and obvious surface rec on struc-tion and the accumulation of high-valence Co species can be identified,proving the crucial role of pre-oxidation process in boosting the OER catalysis.This work proposed a un iversal approach for the rapid,scalable and con trollable fabricati on of the PBA-based materials,and the elucidation of the pre-oxidation process in facilitating the OER catalysis may provide useful guidanee for designing and optimizing advanced catalysts for energy-related electro-oxidation reactions in the future.Wenbin Sun Zimeng Wei Jindi Qi Luyao Kang Jiechen Li Junfeng Xie Bo Tang Yi Xie 2021Chinese Journal of Chemistry2021,39,9:1
3LDH层间限域生长PBA催化PMS降解磺胺嘧啶研究显示文摘为了探讨PBA-LDH/PMS体系对磺胺嘧啶的降解性能、影响因素以及机理,运用共沉淀法制备出Mg/Al–LDH水滑石,再利用Na Cl-HCl法在氮气保护下去除Mg/Al–LDH层间部分的CO32-,使得PBA前驱物[Co(CN)6]3-更易置换LDH层间的Cl-,最后在LDH层间生成钴普鲁士蓝衍生物Co(II)-Co(III) PBA,形成复合物PBA-LDH,与PMS(Peroxymonosulfate,过硫酸氢钾)组成PBA-LDH/PMS非均相催化体系,产生硫酸根自由基,用于降解PPCPs类污染物磺胺嘧啶。结果表明,相较于在LDH限域层间之外形成的普通PBA,限域生长的PBA-LDH/PMS体系对SDZ具有更高的降解速率。PBA-LDH/PMS体系在p H=3.0~9.0、催化剂投量为0.05 g/L的情况下,SDZ在10 min内能降解80%以上。循环试验表明,在4次循环试验过后,PBA-LDH/PMS体系对SDZ的降解效果仍能维持在80%以上。施周 吴子豪 邓林 2020安全与环境学报2020,20,5:0
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