ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
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IF 11.357
Yixin Huang,Jing Zou,Jinbin Lin,Haoyu Yang,Mengyun Wang,Jiawen Li,Wei Cao,Baoling Yuan,Jun Ma
The activation of peroxydisulfate (PDS) by organic compounds has attracted increasing attention. However, some inherent drawbacks including quick activator decomposition and poor anti-interference capacity limited the application of organic compound-activated PDS. It was interestingly found that 2,2′-azino-bis (3-ethylbenzothiazoline-6-sulfonate) (ABTS) could act as both activator and electron shuttle for PDS activation to enhance diclofenac (DCF) degradation over a pH range of 2.0–11.0. Multiple reactive species of ABTS•+, •OH, and SO4•– were generated in the PDS/ABTS system, while only ABTS•+ and •OH directly contributed to DCF degradation. ABTS•+, generated via the reactions of ABTS with PDS, SO4•–, and •OH, was the dominant reactive species of DCF degradation. No significant decomposition of ABTS was observed in the PDS/ABTS system, and ABTS acted as both activator and electron shuttle. Four possible degradation pathways of DCF were proposed, and the toxicity of DCF decreased after treatment with the PDS/ABTS system. The PDS/ABTS system had good anti-interference capacity to common natural water constituents. Additionally, ABTS was encapsulated into cellulose to obtain ABTS@Ce beads, and the PDS/ABTS@Ce system possessed excellent performance on DCF degradation. This study proposes a new perspective to reconsider the mechanism of activating PDS with organic compounds and highlights the considerable contribution of organic radicals on contaminant removal.
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高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 32
·15789-15796
·
IF 9.931
Jiali Sheng,Jiahui Kang,Zhixiong Hu,Yan Yu,Xian-Zhu Fu,Rong Sun,Ching-Ping Wong
Exploring effective electrocatalysts is in urgent demand to boost their large-scale applications for direct ethanol fuel cells. Herein, for the first time, we report nanoparticle-assembled Pd nanocages with efficient catalytic activity towards ethanol electrochemical oxidation. The catalysts are prepared from the second template of a nanosheet surface of amorphous Co(OH)2 octahedral nanocages, which are prepared from the original template of octahedral Cu2O. These Pd octahedral nanocages exhibit a porous rough surface, which consists of smaller Pd nanoparticles, endowing them with highly active surface area and many active sites. For the electrochemical oxidation of ethanol, the Pd nanocages demonstrate superior activity (3765 mA mgPd−1), 4.8 times and 5.9 times those of commercial Pd/C and Pd nanocatalysts, respectively, prepared directly from an octahedral Cu2O original template. Furthermore, the Pd nanocages demonstrate excellent long-term durability.
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高影响因子
JOURNAL OF CATALYSIS
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2017
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IF 6.844
Min Wang,Jianmin Lu,Lihua Li,Hongji Li,Huifang Liu,Feng Wang
Selective oxidative cleavage of C C bond is pivotal for producing functionalized molecules, useful for organic synthesis and biomass utilization. We herein report the oxidative C(OH) C bond cleavage of secondary alcohols to acids over a copper/1, 10-phenanthroline complex with molecular oxygen as the oxidant. A wide range of secondary alcohols are converted into acids with up to 98% yields. More interestingly, it is effective for breaking up lignin model systems into acids, which is rarely achieved in previous studies. Density functional theory (DFT) calculations indicate a copper-oxo-bridged oxygen dimer is the active species for the C H bond cleavage which is the rate-determining step for C C bond.
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高影响因子
GREEN CHEMISTRY
·
2025
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IF 9.2
Xiaoqian Chang,Yunpeng Xu,Chun-Liang Hou,Ruihan Wang,Xiaoyang Chang
Upgrading plastic waste into high-value chemicals and achieving recycling is of great significance for sustainable development. Herein, we report a green, mild, solvent- and metal-free catalytic approach that uses hydroxyl-functionalized ionic liquids to induce the cleavage of C-O and O-H bonds in polyethylene glycol (PEG), successfully converting PEG into ethylene glycol diester. Through experiments, NMR analysis and DFT calculations, we find that the anion and cation of [HO-EtMIm][OTf] can respectively act as hydrogen bond acceptors and donors to activate the O-H and C-O bonds in PEG, as well as the C=O double bond in benzoic anhydride. Subsequently, the activated hydroxyl O atom in PEG can attack the carbonyl C atom in benzoic anhydride through nucleophilic action, and the activated O atom in benzoic anhydride can also attack the C atom in PEG through nucleophilic action, thereby undergoing depolymerization and forming new C-O bonds, ultimately generating the target product. This mechanism clearly demonstrates the importance of unique confinement effect of ionic liquids, which is achieved through spatial confinement, electrostatic stabilization, directional activation, and hydrogen bonding synergy, providing corresponding innovative support for future research.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Zhengda Lin,Yijun Liu,Zhongming Zhang,Jie Yao
In this study we used a high-temperature steam-induced hydrolysis method to obtain a fluorinated OH/SiO 2 -TiO 2 /polyethersulfone (PES) composite hollow fiber membrane for CO 2 capture. The purpose of grafting SiO 2 and TiO 2 on the surface of PES by hydrolyzing silicon precursors and titanium precursors at high temperature, is to improve the alkali corrosion resistance and hydrophobicity of the PES membrane. The OH/SiO 2 -TiO 2 /PES composite hollow fiber membranes prepared by the high-temperature steam-induced hydrolysis method and the graft coating method were measured by SEM, EDS , FTIR, WCA, AFM , XRD and XPS in order to characterize the morphology and structure of the prepared membranes. In the CO 2 /CH 4 separation performance test experiment, the OH/SiO 2 -TiO 2 /PES membrane prepared by the high-temperature steam hydrolysis method showed better separation performance than the original PES membrane. The effects of absorbent flow rate, absorbent concentration and feed gas flow rate on CO 2 flux and CO 2 /CH 4 were selectivity investigated. When the flow rate of the absorbent (DEA) reached 16 L/h, the flow rate of the feed gas (CO 2 /CH 4 = 40 : 60) was 30 ml/min, the concentration of the absorbent was 1 mol/L, The CH 4 concentration was 99.88 % and the optimal separation factor was as high as 554.89. In general, the results obtained in this work may provide promising insights into the use of fluorinated OH/SiO 2 -TiO 2 /PES composite membranes for carbon capture and CO 2 /CH 4 separation in GLMC application.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yujiao An,Xiaowan Li,Zihao Liu,Zhilan Wang,Xiaoquan Lu
Quinones, widely considered as environmental pollutants in wastewater, have been identified as redox-active substances capable of activating persulfate for decontamination purpose. However, the mechanism of peroxydisulfate (PDS) activation by quinones under alkaline conditions remains elusive. In this study, methyl- p -benzoquinone (MBQ) was chosen as a model quinone to elucidate the intrinsic mechanism of activating PDS. The results showed that MBQ/PDS system can effectively degrade atrazine (ATZ) under alkaline conditions (especially at pH 10.5) and achieve simultaneous removal of MBQ. Derivatization analysis, quenching experiments and electron spin resonance tests revealed that the self-transformation product of MBQ, methyl-semiquinone radical (MSQ − ), played a major role in activating PDS while alkali served as an auxiliary activator. Specifically, MSQ − functioned as a mediator in PDS activation, regulating the generation of sulfate radical (SO 4 − ) and hydroxyl radical ( OH), thereby inducing the degradation of ATZ through free radical pathways. Two degradation pathways of ATZ were proposed based on UPLC-Q-TOF-MS analysis and DFT calculation. ECOSAR evaluation indicated MBQ/PDS system can detoxify ATZ, yet it remains imperative to concern the formation of more toxic by-products. Furthermore, MBQ/PDS system exhibited strong resistance to water matrixes (excluding Cl − ) and favorable degradation capabilities towards diverse contaminants. This work broadened the possibility of applying the persulfate system in actual water bodies with alkaline environments, achieving the dual benefit of degrading target contaminants and simultaneously removing the activator quinones themselves, providing a novel “treating pollution with waste” water treatment strategy.
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高影响因子
Journal of Energy Storage
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2025
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IF 9.8
Yuan Yao,Xikun Tian,Jun Yan,Changying Zhao
In light of the widespread adoption of novel energy sources, there is a pressing need for the rapid development of long-term energy storage technologies. While most existing energy storage technologies are prohibitively expensive, the thermochemical energy storage (TCES) system based on CaO/Ca(OH)₂ offers a high storage density of 1400 kJ/kg, low costs, and excellent cycle stability. The choice of expanded graphite (EG) as the matrix is based on its outstanding thermal conductivity and rich microstructure, which enhance heat and mass transfer. This study focuses on the thermochemical properties of Ca(OH)₂ doped by expanded graphite with stable morphology. Five samples with EG contents were synthesized, and characterized with regard to their microstructures, and their thermal and physical properties examined. Additionally, a reaction kinetic analysis of the thermal decomposition process was conducted. The results indicate that the composite with 9 % EG content stands out as the optimal thermal storage material, exhibiting a thermal conductivity of 2.5 W/(m·K), almost three times that of pure material. The activation energy of the composite was calculated to be 166.9 kJ/mol and the pre-exponential factor is 5.5 × 10 11 1/s which is two orders of magnitude higher than the pure. Furthermore, the composite demonstrated exceptional stability during cyclic performance tests, maintaining a conversion rate of 70 % after 10 cycles, confirming its reliability. In conclusion, this research presents a novel approach for the large-scale, low-cost application of TCES in CaO/Ca(OH)₂ systems.
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高影响因子
Journal of Materials Chemistry A
·
2025
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IF 9.5
Zhijian Chen,Zhenghui Ma,Wenlin Yang,Guoli Fan,Baoming Ren,Feng Li
Due to the high energy barrier of C-C coupling and the intense competition from by-products, achieving superior ethylene selectivity in electrochemical CO2 reduction reaction (eCO2RR) remains challenging. Herein, we reported a distinctive Cu-based electrocatalyst fabricated from a three-dimensional (3D) tentacle-like Cu2(OH)2CO3 precursor. After electrochemical activation, abundant surface structural hydroxyls chemically bonded to Cu+ species (Cu+-OH structures) formed on the resulting Cu-based electrocatalyst. Such structural hydroxyl-rich Cu-based catalyst exhibited excellent eCO2RR performance, with a Faradaic efficiency (FE) of 43.7% for ethylene (partial current density up to 130.6 mA·cm-2) and a FE of ~70% for C2+ products at -1.5 V vs RHE in a flow cell, far exceeding those over the hydroxyl-deficient Cu-based one. By combining operando spectroscopic analysis with density functional theory calculations, it was unveiled that inherent surface Cu+-OH structures over Cu-based electrocatalysts could result in the electron loss of neighboring active Cu0 sites, which was favorable for the creation of crucial *COH and *OCCOH intermediates and thus the formation of ethylene product. Consequently, dual reaction pathways for the eCO2RR based on both key *COH and *CHO intermediates coexisting on the Cu-based electrocatalyst with abundant Cu+-OH structures powerfully boosted electrochemical CO2 reduction to produce ethylene. This work presents an innovative strategy for the construction of Cu-based electrocatalyst rich in structural hydroxyls and highlights the crucial role of inherent Cu+-OH structures in switching the formation of intermediates to boost ethylene production in the eCO2RR.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2017
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IF 3.582
Hao Xu,Songsong Li,Lei Ge,Changcun Han,Yangqin Gao,Dongsheng Dai
Efficient separation of photo-generated electrons and holes is a crucial aspect for photocatalytic hydrogen evolution . Herein, novel plate-like Co(OH) 2 decorated TiO 2 nanosheets for photocatalytic water splitting were synthesized by a facile in-situ synthetic method. The results of X-ray diffractometry (XRD), transmission electron microscope (TEM), UV–Vis diffusion reflectance spectroscopy (DRS) and X-ray photoelectron spectroscopy (XPS) indicate the successfully incorporation of Co(OH) 2 co-catalysts onto the surface of TiO 2 nanosheet photocatalysts . Further photocatalytic hydrogen evolution experiments illustrate that all Co(OH) 2 decorated TiO 2 samples show higher rate of hydrogen production performance than pure TiO 2 sample and the composite sample with Co(OH) 2 loading amount of 0.5mol% presents the highest photocatalytic hydrogen production activity of 746.93 μmol g −1 ·h −1 . It is indicated that plate-like Co(OH) 2 particle act as an electron collector, which leads to photo-generated electrons transfer from TiO 2 to Co(OH) 2 , and therefore enhance the photocatalytic activity . Based on above results, a possible mechanism is proposed and further verified by surface photovoltage spectra (SPV).
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高影响因子
Nanomaterials
·
2019
·Vol. 10
·期 1
·53
·
IF 4.034
Yuanyuan Li,Xiaofang Tian,Yaoqiong Wang,Qimei Yang,Yue Diao,Bin Zhang,Dingfeng Yang
Using solar energy to remove antibiotics from aqueous environments via photocatalysis is highly desirable. In this work, a novel type-II heterojunction photocatalyst, MgSn(OH)6/SnO2,was successfully prepared via a facile one-pot in situ hydrothermal method at 220 °C for 24 h. The obtained heterojunctions were characterized via powder X-ray diffraction, Fourier-transform infrared spectroscopy, transmission electron microscopy, and ultraviolet-visible diffuse reflectance spectroscopy. The photocatalytic performance was evaluated for photodegradation of tetracycline solution under ultraviolet irradiation. The initial concentration of tetracycline solution was set to be 20 mg/L. The prepared heterojunctions exhibited superior photocatalytic activity compared with the parent MgSn(OH)6and SnO2compounds. Among them, the obtained MgSn(OH)6/SnO2heterojunction with MgCl2·6H2O:SnCl4·5H2O = 4:5.2 (mmol) displayed the highest photocatalytic performance and the photodegradation efficiency conversion of 91% could be reached after 60 min under ultraviolet irradiation. The prepared heterojunction maintained its performance after four successive cycles of use. Active species trapping experiments demonstrated that holes were the dominant active species. Hydroxyl radicals and superoxide ions had minor effects on the photocatalytic oxidation of tetracycline. Photoelectrochemical measurements were used to investigate the photocatalytic mechanism. The enhancement of photocatalytic activity could be assigned to the formation of a type-II junction photocatalytic system, which was beneficial for efficient transfer and separation of photogenerated electrons and holes. This research provides an in situ growth strategy for the design of highly efficient photocatalysts for environmental restoration.
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高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122405
·
IF 7.5
Xiangwu Meng,Liangji Xu,Jianjun Li,Xuekai Wang,Junshu Wu
Loofah sponge carbon (LOC) was employed as a three-dimensional scaffold and magnetized through alkaline hydrothermal treatment followed by co-precipitation to obtain magnetic loofah sponge carbon (MLOC). Subsequent lanthanum incorporation produced La₃-MLOC, which integrates a hierarchically porous architecture with magnetic separability for phosphate removal from complex waters. La₃-MLOC delivered a Langmuir capacity of 117.32 mg/g at pH 3 and showed rapid uptake across pH 3–6, achieving > 90% removal within 15–40 min while maintaining good tolerance to common coexisting ions. Kinetic fitting (PSO and Avrami, n ≈ 0.82) suggests a predominantly site-specific chemisorption pathway. Microscopic and spectroscopic analyses support La–OH-mediated hydroxyl displacement/inner-sphere complexation, accompanied by partial LaPO₄ precipitation. The sorbent retained high performance over four adsorption–desorption cycles (removal about 92%; desorption about 77%). When evaluated using real effluent from a coal-mining subsidence outfall, La₃-MLOC enabled low-level phosphate polishing to Class III targets at low dosage and short contact time, with an estimated treatment cost of 0.341 USD/g, indicating its potential for end-of-pipe phosphate control and resource-oriented management.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 9.2
Lin Wu,Lixiang Li,Han Zhang,Hongwei Zhao,Qingdong Li,Xueyuan Zhang,Baigang An
Spintronic catalysis remains largely unexplored for the oxygen evolution reaction (OER). Herein, we propose a novel spin-control strategy by constructing an oriented, 1D core-shell CoB@Ni(OH) 2 nanochain architecture. The spin-ordered amorphous ferromagnetic (FM) CoB core effectively induces spin polarization in the antiferromagnetic (AFM) Ni(OH) 2 shell via FM@AFM coupling. Combined experimental and theoretical analyses reveal that an applied magnetic field (MF) induces spin alignment in Ni(OH) 2 . This MF-guided spin alignment triggers directional Ni orbital splitting, promotes d-charge accumulation at Ni–O sites, and activates a switch to the highly efficient lattice oxygen mechanism. Consequently, the CoB@Ni(OH) 2 catalyst achieves a low overpotential of 472 mV at 100 mA cm -2 and exhibits stability exceeding 150 h under an MF, markedly outperforming its non-magnetic operation. This work demonstrates that engineering FM@AFM interfaces enables the transformation from spin disorder to spin alignment, opening a new avenue for spin-regulated electrocatalytic material design.
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高影响因子
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