Catalysts
·
2023
·Vol. 13
·期 3
·637
·
IF 3.9
Yuling Wang,Yun Chen,Xinlei Ding,Jianwei Song,Gaixia Wei,Hengwei Dai,Hanyang Wang,Yadong Liu,Guangmei Bai,Wenge Qiu
In order to reduce the noble metal palladium dosage in the preparation of CL-20 so as to reduce its production cost, several carbon supports were prepared successfully using the hydrothermal carbonization method in the absence or presence of urea using microcrystalline cellulose (MC) as the carbon source, and the corresponding Pd(OH)2/C catalysts were fabricated using the deposition–precipitation method, which showed high activity in the debenzylation reaction of hexabenzylhexaazaisowurtzitane (HBIW) and tetraacetyldibenzylhexaazaisowurtzitane (TADB). It was found that all the catalysts showed a high efficiency in the debenzylation of HBIW, indicating that the structure of the used carbon supports had a limited impact on the catalyst performance in this reaction. On the contrary, the activities of the catalysts in the debenzylation of TADB were quite different. The results of the nitrogen sorption isotherm measurement (BET), scanning electron microscope (SEM), scanning transmission electron microscopy (STEM), powder X-ray diffraction (XRD), element analysis and temperature programmed desorption (TPD), as well as X-ray photoelectron spectra (XPS) characterizations of the supports and catalysts, showed that the relatively high activity of Pd/HTC in the debenzylation of TADB was related to the high Pd dispersion and novel mesoporous structure, while the further higher activity and stability of Pd/HTC-N1:1in the same reaction were related with its high Pd dispersion, high total oxidized Pd species, and high surface pyridinic N contents as well as the eggshell distribution of Pd species on the support.Keywords:nitrogen doping carbon support;Pd(OH)2/C catalyst;hydrogenolytic debenzylation
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xincheng Jiang,Junyi Jiang,Guoyou Huo,Jiaxi Guo,Qiquan Zheng,Hong Li,Huaili Zheng
Effectively removing both soluble antibiotics and insoluble oils from wastewater is a significant challenge. To address both the problems, we synthesized a three-dimensional (3D) porous water treatment material. It can be converted from antibiotic removal mode to oil removal mode by simple surface performance regulation. This approach achieved a high removal rate for ciprofloxacin (CIP) and good separation efficiency for oil/water mixtures. Initially, Co 2 CO 3 (OH) 2 nano-needles were fixed on Ni foam to synthesize Co 2 CO 3 (OH) 2 @Ni foam-1, which had a high CIP removal rate (93.59 % at pH 7.0) and a certain anti-interference ability. To assess the CIP removal performance, the environmental impact, economic benefit and energy consumption (3E) triangle model was established and the optimal operating point was selected. Characterization experiments demonstrated that the removal of CIP was attributed to the mechanisms of surface complexation, electrostatic attraction, cation bridging, precipitation and flocculation . Subsequently, Co 2 CO 3 (OH) 2 @Ni foam-2 was obtained by hydrophobic modification, which exhibited separation efficiencies above 93.5 % for a series of different oil/water mixtures. Co 2 CO 3 (OH) 2 @Ni foam series materials are easy to prepare and possess effective pollutants treatment efficiency, thus providing a new strategy for developing multi-functional water treatment materials and a novel approach for the treatment of soluble antibiotics and insoluble oils in wastewater.
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GIANT
·
2022
·
IF 0
Yifan Jia,Weiwen Yuan,Mengmeng Xu,Congyi Yang,Lei Chen,Shuo Wang,Paul D. Topham,Guoxuan Luo,Mo Wang,Yong Zhang,Guihua Jiang,Qianqian Yu,LinGe Wang
Magnetic resonance imaging (MRI)-active polymers exhibit unique advantages for in vivo diagnosis. Here, in order to endow electrospun fibers with long-term T 1 positive MRI visibility, MRI contrast agent (CA), Gd(OH) 3 , is introduced in a new, extremely convenient method. Crucially, GdCl 3 is reacted with NaOH in situ during electrospinning, with flexibility to deliver both well-dispersed and aggregated Gd(OH) 3 clusters within a poly(ethylene terephthalate) (PET) matrix. T 1 and T 2 relaxivities of Gd(OH) 3 in PET nanofibers are studied. Well-dispersed Gd(OH) 3 (sub-nanometer in size) exhibits 34 times higher T 1 relaxivity than aggregated nanoparticles when embedded within the fibers. The morphology, structure, magnetic properties, tensile properties, imaging performance and biosafety of the PET/Gd(OH) 3 composite fibers are evaluated to identify the optimum conditions to produce new materials with balanced properties, excellent in vivo positive contrast and approximately 139 days imaging lifetime. Comparing this sample with a commercial CA, only 0.32 wt.% Gd loading is needed to attain similar MRI signal intensity. In summary, PET/Gd(OH) 3 long-term MRI-active fibers show great potential for future biomedical applications and the study also provides a promising new general strategy to enhance the MRI T 1 positive contrast of electrospun fibers of a whole host of other systems.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Chaojie Lyu,Jiarun Cheng,Kaili Wu,Jiwen Wu,Ju Hao,Yuanyuan Chen,Huichao Wang,Yunguo Yang,Ning Wang,Woon-Ming Lau,Jinlong Zheng
Transition metal-based electrocatalysts are the promising candidates to substitute noble metal-based catalysts for water electrolysis, owing to its abundant earth reserves and inexpensive fabrication costs. Interface engineering and cation doping engineering are verified as the effective methods to improve the sluggish electrocatalytic performance of transition metal-based electrocatalysts. Here, we synthesized a self-supported heterostructure of Ce doped Co(OH) 2 nanosheets/CoP nanowires on the support of nickel foam (Ce-Co(OH) 2 /CoP/NF) by simple hydrothermal method , low-temperature phosphorization method. The Ce atom doping can lead to lattice distortion and abundant superficial defects on crystal surface, which will generate more active sites and faster charges transformation. The heterointerface between Ce-Co(OH) 2 and CoP also can lead to electronic structure modulation at interface domain, which not can induce much fresh active sites in this area, but can optimize the active sites to the optimal state for superior catalytic activity. Benefitting from these, it only needs the overpotentials of 253 and 56 mV to realize 10 mA/cm 2 for OER and HER under 1 M KOH solution, which is much enhance than single-phased samples. As the bifunctional electrocatalyst for two-electrode system, it merely requires 1.53 V to attain 10 mA/cm 2 in 1 M KOH, and it also exhibits outstanding overall water splitting performance in alkaline natural electrolyte, along with excellent catalytic long-time durability. In addition, the Ce-Co(OH) 2 /CoP/NF-based electrolyzer also could achieve energy-saving hydrogen production, and simultaneously oxidative degradation of organic materials or biomass upgrading at anode under lower voltages. This work paves a novel idea to fabricate high-efficient bifunctional electrocatalysts for energy-saving H 2 production.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Lijing Zhang,Jiaqi Han,Yuchao Wang,Wenbo Yang,Shengyang Tao
Achieving a room-temperature Suzuki–Miyaura coupling (SMC) with high efficiency is of great significance to the development of low-carbon organic synthesis. Nevertheless, it is still a great challenge to construct a promising nanocatalyst with high activity for room-temperature SMC reaction. In this paper, a strong alkaline-supported nanocatalyst Pd/Mg(OH)2/MgO–ZrO2 was rationally developed based on MgO–ZrO2 hybrid nanofibers. Physicochemical characterizations present that the in situ conversion of MgO to Mg(OH)2 on the surface of the nanofibers results in a great increase in surface alkalinity of the carrier. The strong alkalinity can greatly accelerate the oxidation addition and transmetalation of the SMC process, resulting in the obvious reduction of activation energy of the reaction (Ea = 9.0 kJmol–1 for Ph–Br). The coupling conversion can reach up to 100% at room temperature within 8 min with a maximum TOF > 6516 h–1. It also shows an excellent performance in substrate applicability and chlorobenzene activation. The rational design of a high-basicity catalyst for room-temperature SMC will be a rewarding attempt for the development of low-carbon green organic synthesis.
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ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Huasheng Lai,Gongke Li,Zhuomin Zhang
Improving the speediness of complex sample analysis has attracted much research interest in analytical science. In this work, an enrichment-sensing all-in-one strategy was presented for rapid surface-enhanced Raman spectroscopy (SERS) analysis of purine components by using the La(OH)3-Au@AgNPs nanocomposite. Two-dimensional (2D) La(OH)3 nanosheets with nanothickness and accessible active sites not only acted as efficient media for the rapid enrichment of analytes but also provided flat planes for the intensive decoration of Au@AgNPs nanoparticles to amplify the SERS signals of adsorbed analytes. The nanocomposite could realize the rapid enrichment-sensing of purine components in 1 min, including mercaptopurine, thioguanine, adenine, and purine. Subsequently, the surface adsorption behaviors were explored by density functional theory and the enhancement mechanisms were simulated by the finite-difference time-domain method. Moreover, the nanocomposite also exhibited good SERS performances with relative standard deviations (RSDs) of uniformity less than 6.5% (n = 23), RSDs of batch-to-batch stability less than 7.3% (n = 9), and long-term stability over 9 weeks with RSDs within 6.6%. Finally, the enrichment-sensing strategy was applied for the rapid SERS analysis of two projects: mercaptopurine in tablets and adenine in beers with detection limits of 6.0 and 0.76 μg/L and spiked recoveries of 90.9–100 and 84.2–101%, respectively. Benefiting from the high-performance enrichment medium and closely packed plasmonic nanoparticles, the enrichment-sensing all-in-one strategy possesses great potential for rapid on-site detection in food safety and pharmaceutical analysis.
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PubMed
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PROGRESS IN ORGANIC COATINGS
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2021
·
IF 5.161
Hua-Rong Zhao,Zan Liu,Zhi-Lin Cheng
The interfacial issue of nanomaterials-filled epoxy coating has seriously restrained its ongoing progress in actual application. In this paper, we reported a novel design for the robust anti-corrosion and anti-friction performance epoxy coating system based on the self-synthesized 2D Co 2 (OH) 2 BDC nanosheets with the native compatible interface compatibility and non-conductivity. The composite epoxy coatings(EP) were intensively characterized by a series of spectral instruments. The influence of the filling content of 2D Co 2 (OH) 2 BDC nanosheets to the interface structure of epoxy coating was probed by the microcosmic change. Lastly, the anti-corrosive, mechanical and tribological behaviors of the composite epoxy coatings were extensively investigated. At the optimal filling content of 0.6 wt.%, the low frequency impedance modulus of the 2D Co 2 (OH) 2 BDC/EP was increased by about 2 orders of magnitude relative to the neat epoxy coating. Moreover, the friction coefficient of the 2D Co 2 (OH) 2 BDC/EP was decreases by 20 % due to the layered structure of nanosheets derived from the weak van der Waals force, while the hardness and Young's modulus were separately increased by 41 % and 83.3 % as a result of the better compatibility and dispersion in epoxy matrix to a certain degree.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Xi Tao,Poyueh Pan,Taobo Huang,Long Chen,Haodong Ji,Juanjuan Qi,Fengbin Sun,Wen Liu
Sulfachloropyridazine (SCP) was commonly used as a broad-spectrum sulfonamide antibiotic and hard to be removed through traditional sewage treatment process. In this study, we developed a simple and controllable strategy to realize in-situ construction of Co(OH) 2 nanoparticles decorated urchin-like WO 3 (Co(OH) 2 /WO 3 ), which could efficiently remove SCP through peroxymonosulfate (PMS) activation. Some tiny nanoparticles of Co(OH) 2 decorated on the spines/nanorods or surfaces of urchin-like WO 3 by transmission electron microscopy (TEM) analysis. The obtained 10 wt% Co(OH) 2 /WO 3 realized completely removal of SCP (degradation efficiency 100%) with a high reaction rate constant ( k 1 ) of 0.88 min −1 within 3 min at optimal pH 7. That was because the urchin-like WO 3 with numerous adsorption functional groups on its surface ( e.g. , W = O and –OH bonds) could adsorb the Co 2+ easily to form CoOH + , which was perceived the rate-limiting step for PMS activation and generating radicals. Radical quenching experiments indicated that SO 4 •− played a more significant role than HO • radicals. Density functional theory (DFT) calculation revealed that the atoms of SCP with high Fukui index ( f − ) were active sites, which preferred to be attacked by the electrophilic SO 4 •− and HO • radicals. The toxicity of the intermediates by SCP degradation was evaluated by quantitative structure–activity relationship (QSAR) prediction through Toxicity Estimation Software Tool (T.E.S.T.). The possible degradation pathway and catalytic mechanism for SCP removal were proposed. Considering the good catalytic properties of Co(OH) 2 /WO 3 -PMS, the material will show great application potential in the removal of emerging contaminants in water.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Hairus Abdullah,Riski Titian Ginting,Refi Ikhtiari,Noto Susanto Gultom,Hardy Shuwanto,Dong-Hau Kuo
Configurational entropy composites of In-doped Zn(O,S)/Zn-doped In(OH) 3-x S x has been synthesized with a one-step hydrothermal method and carefully characterized with XRD , XPS , SEM, TEM, DRS , PL , EIS , TPC , CV , and MS analyses. The composites were prepared with different sulfur amounts to obtain the optimum performance of visible-light photocatalytic HER . The primary phases of ZnS and In(OH) 3 were formed after the hydrothermal process. However, the results indicated In and O were doped into ZnS lattice and induced lower bandgap values (~2.71–2.84 eV) which are active in visible-light illumination. Simultaneously, the excess Zn and S were also doped to In(OH) 3 with lower bandgap values (~3.38–4.63 eV). The variation of bandgap values is due to the hybridization of In 5s5p to Zn 4s4p and O 2p to S 3p orbitals. As a result, In-doped Zn(O,S) and Zn-doped In(OH) 3-x S x will be a visible-light active material for photoreaction and a favorable phase for electron transfer , respectively. Furthermore, it is also related to a possible antisite-defect formation with I n Z n + to help the electron trapping and enhance the photocarrier separation, leading to an efficient photocatalytic activity . ZI-S1 with additional 5-mmol thioacetamide was found as the catalyst with the highest HER performance which achieved 730 μmol/g·h under visible-light illumination. A plausible photocatalytic HER mechanism is discussed and proposed in this work.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Zhong-Shuai Zhu,Xiao-Jie Yu,Jin Qu,Ya-Qiong Jing,Yasmine Abdelkrim,Zhong-Zhen Yu
Low crystalline flowerlike cobalt silicate hydroxide (Co 3 (Si 2 O 5 ) 2 (OH) 2 , CoSiO x ) is synthesized by a one-pot hydrothermal approach. Abundant highly active Co OH + is preformed on the surface of CoSiO x , while the low crystallinity of CoSiO x leads to the formation of active 1 O 2 caused by the generation of oxygen vacancy in the valence change cycle between Co 2+ and Co 3+ . The optimal CoSiO x with a high specific surface area of 665.2 m 2 g −1 could expose surface Co OH + , thus rapidly activate peroxymonosulfate (PMS) and accelerate catalytic efficiencies. As a result, at least 11 kinds of organic pollutants could be degraded with 33–242% higher efficiencies than reported. In addition to the common SO 4 - and OH, large amounts of active 1 O 2 endow the CoSiO x /PMS system with superb catalytic performances in diverse conditions, suggesting the excellent adaptability for practical usage. This work provides a new protocol to advance the PMS activation process for high-performance cobalt based heterogeneous catalysts.
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 39
·19201-19209
·
IF 9.931
Guoqiang Liu,Zhongti Sun,Xian Zhang,Haojie Wang,Guozhong Wang,Xiaojun Wu,Haimin Zhang,Huijun Zhao
Electrocatalytic water splitting has been widely accepted as an environmentally friendly approach to generate clean H2. However, the sluggish oxidation half reaction, namely, the oxygen evolution reaction (OER), usually requires a high overpotential, which is the obstacle to high-efficiency overall water splitting to generate H2. Herein, we report the preparation of ultrathin nanosheet array Ni3S2 with a 9–14 nm nanosheet thickness grown directly on a commercial Ni foam substrate (Ni3S2/NF) by in situ vapor-phase hydrothermal (VPH) transformation of the nanosheet array structure Ni(OH)2/NF precursor. As a multifunctional electrocatalyst, the as-fabricated Ni3S2/NF-2 (VPH time of 2 h) displays excellent electrocatalytic activities toward the hydrazine oxidation reaction (HzOR) with a potential of 0.415 V (vs. RHE) to deliver a current density of 100 mA cm−2, an OER with an overpotential of 425 mV obtaining the same current density, and a hydrogen evolution reaction (HER) with an onset potential of −0.05 V (vs. RHE) in 1.0 M KOH media. A two-electrode system is therefore constructed using Ni3S2/NF-2 as both the anode and cathode, capable of achieving 100 mA cm−2 at 0.867 V in 1.0 M KOH with 0.2 M hydrazine. Density functional theory (DFT) calculations reveal that the adsorption of N2H4 molecules on the Ni3S2 (110) is more thermodynamically favourable than H2O, thus contributing to the high HzOR activity.
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Environmental Science-Nano
·
2018
·Vol. 5
·期 11
·2570-2578
·
IF 6.087
Xinwen Ou,Xueming Liu,Weizhen Liu,Wencong Rong,Jingyuan Li,Zhang Lin
The surface defects of adsorbents are generally considered to be the active sites for adsorbates, and the adsorption behaviors of a variety of pollutants in wastewater are strongly influenced by the surface defects of the adsorbents. With simple chemical and structural properties, nano-Mg(OH)2 exhibits a high adsorption affinity and selectivity to heavy metals from wastewater. The insight into the surface complex structures of heavy metals on the Mg(OH)2 surface is fundamental for both the mechanism and application of defective adsorbents in wastewater treatment. In this study, the impact of surface defects of Mg(OH)2 nanoplates on the structure, energy, and adsorption amounts of toxic heavy metal oxyanions (HAsO42− and CrO42−) was investigated by combining the first-principles calculations and batch experiments. The first-principles calculations illustrated that the heavy metal oxyanions can be steadily incorporated into the surface defects to form inner-sphere complexes. The incorporated heavy metal oxyanions have strong charge–charge and chemical bonding interactions with the surface defect sites, which are much stronger than the hydrogen bonding interactions with the surface OH sites. Moreover, the adsorption affinity of surface defects towards heavy metal oxyanions is stronger than that towards other oxyanions (e.g. SO42− and NO3−), indicating the high adsorption selectivity of heavy metal oxyanions over other oxyanions. Batch adsorption experiments verified that the adsorption of defect-rich Mg(OH)2 adsorbents towards heavy metal ions, e.g., As(V) and Cr(VI), was favorable even under the condition of low concentration (mg L−1 level). These findings reveal the significance of surface defects of Mg(OH)2 for extracting As(V) and Cr(VI) from low-concentration solutions. The proposed strategy of surface defect-fabrication should provide a useful insight into designing effective adsorbents for the selective extraction of heavy metal oxyanions at low concentration.
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