Catalysis Science & Technology
·
2025
·
IF 4.2
Yifan Zhang,Jiaying Liu,Shiwei Wang,Zhihao Yu,Haojian Zhang,Dong Wang,Lin Zhu,Chunzheng Wu,Hongbo Yu
Modifying noble metal catalysts with transition metal oxides (MO x ) can markedly enhance catalytic performance through synergistic effects, yet precise spatial colocalization of active metal and promoter phases remains challenging. Here, we report the synthesis of KIT-6 supported Pd-MO x (M = Fe, Co, Ni) hybrid nanostructures via in situ transformation of bimetallic PdM nanoparticles under controlled thermal conditions. The resulting Pd-MO x /KIT-6 catalysts displayed superior activity and selectivity in the selective hydrogenation of acetophenone to 1-phenylethanol compared with monometallic Pd/KIT-6. Among them, Pd-CoO x /KIT-6 (Pd/Co=1:1) achieved the highest performance, with 99.7% acetophenone conversion and 98.2% selectivity, and demonstrated broad applicability for hydrogenating diverse ketones. Structural and kinetic studies revealed that interfacial Pd-CoO x sites play a pivotal role: Pd domains efficiently dissociate H 2 , while CoO x species enhance acetophenone adsorption. This synergistic interface-driven mechanism provides a general and costeffective strategy for the selective hydrogenation of multifunctional substrates.
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JOURNAL OF HAZARDOUS MATERIALS
·
2026
·
IF 10.6
Hang Xu,Wenhui Zhang,Sicheng Zhu,Bingyu Shen,Xinyu Li,Bingqi Jiang,Lianhong Wang,Philippe F.X. Corvini,Max M. Häggblom,Rong Ji
Transformation of bisphenol compounds during nitrogen removal processes in wastewater treatment plants, along with the key microbial taxa associated with this transformation, remains poorly understood. In this study, we examined the transformation of a series of alkylbisphenols (ABPs; bisphenol A, bisphenol E, and bisphenol F) and sulfonylbisphenol (bisphenol S) in an enriched nitrifying activated sludge (NAS). While bisphenol S was persistent in the NAS, the ABPs were effectively transformed; however, 14 C-isotope tracing revealed that the majority of BPA (presumably also other ABPs) was retained in the NAS as transformable intermediates and potentially toxic nitroaromatic compounds, with minor mineralization (< 1 %). In total, nine transformation products were identified, including nitrated aromatic compounds and single-ring phenolic compounds. Ammonia‑oxidizing bacteria (AOB), primarily Nitrosomonas , drove abiotic ABP transformation to persistent nitroaromatic products. Heterotrophic bacteria, such as Sphingomonas , Methyloterena , and Comamonas , initiated ABP transformation via type II ipso- hydroxylation and oxidative cleavage, and also mineralized the intermediates formed through the AOB-mediated dealkylative nitration. By integrating batch experiments, HPLC–QTOF-MS/MS, 14 C-tracing, and 16S rRNA gene sequencing, we provide a comprehensive understanding of these complementary transformation pathways and the key microbial taxa involved. Our findings highlight the significant role of AOB-mediated abiotic reactions in ABP transformation, and alarmingly revealed that the traditional nitrogen removal processes using NAS may produce toxic persistent nitroaromatic compounds, thereby leading to unexpected environmental risks.
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WATER RESEARCH
·
2026
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IF 12.8
Yue Wang,Jingyi Lin,Yonghuan Zhao,Weiguang Lv,Bo Liang,Peihua Li,Kaisheng Zhang,Xing-jiu Huang
Tetracycline (TC) is widely detected in natural waters, yet its transformation under environmentally relevant oxidative conditions remains poorly understood, because most previous studies have focused on engineered oxidation systems employing strong oxidants or external energy input. Here we show that humic-like phenolic moieties can act as active mediators to redirect δ-MnO 2 -driven TC transformation from slow direct oxidation to a phenoxy-radical-mediated coupling pathway. Screening of 18 humic-acid model compounds identified acetosyringone (AS) and syringaldehyde (SyrA) as the most effective co-reactants, increasing the apparent rate constants ( k obs ) of TC by about 8.5- and 5.9-fold, respectively. Analyses indicate that TC transformation is governed by syringyl-type phenoxy radicals generated via surface-mediated one-electron transfer on δ-MnO 2 , with reactivity controlled by the fraction of deprotonated phenolic precursors (ArO − ) over a near-neutral pH range. The structure-activity analysis further revealed that ortho‑methoxy and para-carbonyl functionalities favor radical stability and cross-reactivity, whereas para-carboxyl substitution biases the mediator toward self-coupling and unproductive oxidant consumption. These substituent-dependent trends provide molecular-level insight into how humic-like phenolics regulate TC transformation at Mn oxide interfaces.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Mingxue Li,Pijun Duan,Yanru Huo,Jinchan Jiang,Yuxin Zhou,Yuhui Ma,Zhehui Jin,Qiong Mei,Ju Xie,Maoxia He
Recent research revealed inhibition or enhancement of dissolved organic matter (DOM) to the degradation of trace organic contaminants (TrOC) in natural and engineered water systems. Phenols containing acetyl, carboxyl, formyl, hydroxy, and methoxy groups were selected as the model DOM to quantitatively study their roles in the degradation of simple anilines, sulfonamide antibiotics, phenylurea pesticides by sulfate radicals (SO 4 • − ). Experimental results found that p -methoxyphenol inhibited aniline and sulfamethoxazole degradation by thermally activated peroxydisulfate (TAP), while p -acetylphenol slightly promoted aniline degradation. Quantum chemical calculations were applied to study the microscopic mechanism and kinetics of phenols affecting the degradation of aniline pollutants (AN) in three ways: competitively reacting with SO 4 • − , repairing aniline cationic radicals (AN • + ) and phenylaminyl radicals (AN(-H) • ), and generating phenoxy radicals to degrade anilines. Generally, the degradation of sulfonamides and phenylureas prefer to be inhibited by hydroxy- and methoxy-phenols with low oxidation potential ( E ox ), due to their diffusion-limiting reaction with SO 4 • − and rapid back-reduction AN • + with the calculated rate constants of (0.02 − 6.38) × 10 9 M −1 s −1 . Phenols repairing AN(-H) • through H abstraction reaction is speculated to possibly dominate the joint degradation of phenols and anilines by TAP, which has a poor correlation with E ox . This study provides mechanistic insight into the chemical behavior of complex and heterogeneous DOM in complex aqueous environments.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Zhimin Gong,Gaobo Wang,Shuai Shao,Mengjie Wang,Kun Lu,Shixiang Gao
Catalyzed oxidative reactions mediated by enzymes have been proposed as an effective remediation strategy to remove micropollutants. However, enzyme-catalyzed oxidation processes are usually limited to the substrates of phenols and amine compounds. The addition of synthetic redox mediators could extend the types of enzyme-catalyzed substrates. However, the actual applications were hindered by the high cost and potential toxicity of mediators. Here, we discovered a potential HRP-mediator system by exploring the removal of co-existing pollutants amlodipine (AML) and methylparaben (MeP). It was found that MeP served as a redox mediator could efficiently mediate the removal of AML by HRP/H 2 O 2 system. Surface electrostatic potential analysis of AML molecule suggested that MeP radicals (MeP OX ) could abstract hydrogen from the N-H site on dihydropyridine moiety of AML and then be reduced to MeP. By exploring the mediating effects of substances with MeP-like structure, Hirshfeld charge was used to evaluate the mediating efficiency of mediators. For mediating the degradation of AML, when the Hirshfeld charge of mediator radical was around − 0.3000, the mediating efficiency was the highest. This study improved the HRP-mediated system and provided an efficient and green method for the degradation of co-existing pollutants AML and MeP.
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FUEL
·
2020
·
IF 5.578
Xingfei Tang,Wentao Ding,Hao Li
Bio-oil, one of significant renewable energy, was blocked from its direct application by thermodynamic instability due to the high oxygen content, so its deoxygenation needs urgent solution. Avoiding the disadvantages of the traditional catalytic method, such as harsh reaction conditions, potential explosion risk and environmental pollution, we utilize solid-acidic zeolites as low-load Pd-based catalyst supports instead of corrosive acid additives, with polymethylhydrosiloxane (PMHS) as the hydrogen-supplying agent, to achieve efficient hydrodeoxygenation of bio-oil models (carbonyl compounds) under mild conditions. The reaction conditions such as Si/Al ratio of HZSM-5 zeolite, temperature, solvent, and the type of Pd salts precursor are optimized. In particular, we have found that polar protic solvents improve catalytic efficiency by promoting proton transfer in the reaction. In an open-to-air, 97.9% ethylbenzene yield can be obtained for acetophenone conversion under mild conditions (0.5 wt% Pd/HZSM-5(18), 65 °C, 3 h, n-butanol as solvent), which is more efficient and environmental friendly than currently reports. Meanwhile, hydrogenation–dehydration mechanism was proposed, and the Brønsted acid in HZSM-5 promotes the dehydration of the alcohol (rate-limiting step) by efficiently accelerating the removal of hydroxyl groups and the proton transfer of the reaction. Furthermore, the catalytic scheme exhibits the excellent stability (reusable seven times) and versatility. The potential of a green catalytic technology using with PMHS opens attractive opportunities for bio-oil upgrading.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 22
·期 20
·11508-11518
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IF 3.43
Jing Chen,Hanling Yang,Hongquan Fu,Hongyan He,Qiang Zeng,Xuehui Li
Electrochemical oxidation is a promising and effective method for lignin depolymerization owing to its selective oxidation capacity and environmental friendliness. Herein, the electrooxidation of non-phenolic alkyl aryl ether monomers and β-O-4 dimers was experimentally (by cyclic voltammetry, in situ spectroelectrochemistry, and gas chromatography-mass spectroscopy) and theoretically (by DFT calculations) explored in detail. Compared to the reported literature (T. Shiraishi, T. Takano, H. Kamitakahara and F. Nakatsubo, Holzforschung, 2012, 66(3), 303–309), 1-(4-ethoxyphenyl)ethanol showed a distinguishable oxidation pathway, where the resulting carbonyl product surprisingly underwent a bond cleavage on alkyl–aryl ether to ultimately produce a quinoid like compound. In contrast, β-O-4 dimers, like 2-phenoxy-1-phenethanol and 2-phenoxyacetophenone also demonstrated electrochemical oxidation induced by Cβ–O and Cα–Cβ bond cleavages. For the oxidation products, the presence of the Cα-hydroxyl group in dimers was the key to selectively generate aldehyde-containing species under mild electrochemical conditions, otherwise it produces alcohol-containing products following a different mechanism compared to the CαO containing dimers.
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BIOORGANIC & MEDICINAL CHEMISTRY
·
2013
·
IF 2.903
Zhixuan Zhou,Jiaru Zhuo,Sujun Yan,Lin Ma
In this study, twenty 3,5-diaryl-4,5-dihydro-1 H -pyrazole derivatives with hydroxyl(s) ( 1a – 1p , 2a – 2d ) were synthesized and their inhibitory activity on mushroom tyrosinase was examined. The results showed that among these compounds, 1-(5-(3,4-dihydroxyphenyl)-3-(4-hydroxyphenyl)-4,5-dihydro-1 H -pyrazol-1-yl)ethanone 1d was found to be the most potent tyrosinase inhibitor with IC 50 value of 0.301 μM. Kinetic study revealed that these compounds were competitive inhibitors of tyrosinase and their structure–activity relationships were investigated in this article.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Daihong Gao,Denghao Ouyang,Xuebing Zhao
Lignin was oxidized and depolymerized by a direct biomass fuel cell (DBFC) for electricity generation and production of aromatic aldehydes. The yield of aromatic aldehydes could be easily controlled by changing the anodic catalyst, cathodic oxidants and external loading. Cobalt and (VO 2 ) 2 SO 4 were screened as the most suitable anodic catalyst and cathodic oxidant, respectively. A maximum power density of 199.8 mW/cm 2 was obtained under the optimized conditions for electricity generation; however, the yield of the aromatic aldehydes was greatly dependent on the type of lignin used, reaction conditions and the external loading (output voltage) of the DBFC. At a lignin concentration of 0.5 g/L, aromatic aldehydes yield of 7.8 % was obtained at an output voltage of 0.9 V. The formation of aromatic aldehydes was mainly caused by cleavage of β-O-4 linkage and oxidation of side chains by the hydroxyl radicals formed via oxidation of OH – by Co 3+ on the anode.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2023
·
IF 4.4
Tong Shao,Xiaolei Song,Yufeng Jiang,Chenchen Wang,Peng Li,Shihao Sun,Dingzhong Wang,Wei Wei
Among various chemiluminescence (CL) systems, luminol-H 2 O 2 system is used extensively due to its cheapness and sensitivity. Herein, 4-hydroxy-3-methoxybenzaldehyde, known as vanillin, was firstly found to be able to catalyze H 2 O 2 very efficiently to produce • OH and O 2 •− , which can be used to enhance the CL of luminol-H 2 O 2 as Co + . In alkaline aqueous solution, vanillin catalyzed the dissociation of H 2 O 2 into active • OH and O 2 •− radicals and accelerated luminol-H 2 O 2 reaction to emit strong CL signal. Combining the stabilizing function of β-CD, CL intensity of luminol-H 2 O 2 was enhanced further. Thus, dual-signal amplification of luminol-H 2 O 2 chemiluminescence based on the catalyzing function of vanillin and the stabilizing function of β-CD was proposed and its mechanism was explored deeply in the manuscript. Interestingly, vanillin is a highly prized flavor compound broadly used as food additive, however, the excessive intake of vanillin is harmful to human and thus the determination of vanillin is very important. On the basis of the luminol-β-CD-H 2 O 2 /vanillin reaction, a low-cost, rapid and simple CL sensor has been established to detect vanillin. The sensor was able to detect vanillin in the range of 1.0 μM ∼ 75 μM with a detection limit of 0.89 μM (S/N = 3). It can also be used for CL imaging detection with satisfactory results.
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Polymers
·
2019
·Vol. 11
·期 1
·176
·
IF 3.164
Wei Dong,Xuan Wang,Bo Tian,Yuguang Liu,Zaixing Jiang,Zhigang Li,Wei Zhou
Aromatic voltage stabilizers can improve the dielectric properties of cross-linked polyethylene (XLPE); however, their poor compatibility with XLPE hinders their practical application. Improving the compatibility of aromatic voltage stabilizers with XLPE has, therefore, become a new research goal. Herein 1-(4-vinyloxy)phenylethenone (VPE) was prepared and characterized. It can be grafted onto polyethylene molecules during the cross-linking processes to promote stability of the aromatic voltage stabilizers in XLPE. Fourier transform infrared spectroscopy confirmed that VPE was successfully grafted onto XLPE, and effectively inhibited thermal migration. Thermogravimetric analysis showed that the grafted VPE/XLPE composite exhibits a better thermal stability than a VPE/PE blend composite. Evaluation of the electrical properties showed that the breakdown strength and electrical tree initiation voltage of the VPE/XLPE composite were increased by 15.5% and 39.6%, respectively, when compared to those of bare XLPE. After thermal aging, the breakdown strength and electrical tree initiation voltage of the VPE/XLPE composite were increased by 9.4% and 25.8%, respectively, in comparison to those of bare XLPE, which indicates that the grafted voltage stabilizer can effectively inhibit its migration and enhance the stability of the composite material.Keywords:cross-linked polyethylene;grafted voltage stabilizer;breakdown strength;electrical tree initiation voltage
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Food Packaging and Shelf Life
·
2019
·
IF 3.63
Li-Xian Zhu,Qin-Bao Lin,Jia-Yi Li,Hong-Mei Zhu,Hong-Sheng Ma,Huai-Ning Zhong,Jing-Jing Pan
In this study, potassium permanganate (KMnO 4 ) consumption on some key raw materials of food contact paper was analyzed, the content of lignin and total sugar in water simulant for KMnO4 consumption test was analyzed by GC–MS and UV–vis respectively, and the contribution to KMnO4 consumption of the paper samples from lignin and total sugar was investigated. The results have shown that cassava starch has the highest KMnO 4 consumption value among all the starches analyzed, and the KMnO 4 consumption of lignin was significantly greater than that of starches and glucose. KMnO 4 consumption of 15 different commercial paper samples and 10 different commercial fiber molding products were analyzed. The results indicated that KMnO 4 consumption of 12 commercial paper samples were exceeded the limit of 40 mg/kg set forth in GB 4806.8 national food safety standard for food contact paper and paper article. The contribution to the KMnO 4 consumption value of paper samples and fiber mold products from lignin and total sugar in water simulant was from 42% to 94% in most of the samples, lignin and total sugar were two main sources of KMnO 4 consumption in food contact paper. It is known that lignin and total sugar are nature materials and they are non-hazardous, which is not appropriate to set such control limit in the food safety standard, therefore, the limit of KMnO4 consumption for food contact paper and paperboard in GB4806.8-2016 should be revised.
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