PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 19
·13716-13727
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IF 3.3
Caihong Wang,Yong Liu,Fengshen Han,Yongzhe Han,Tianyu Liu,Haitao Ren,Xu Han
Using metal-free catalysts is widely recognized as a promising approach toward wastewater remediation because of the absence of metal leaching. However, the oxidation products involved in the oxidation process and the corresponding mechanisms are still not clear. In this work, N-doped carbocatalysts (CN) were fabricated using as-prepared g-C3N4 and glucose solution, and the reactivity of the as-prepared catalysts was optimized by controlling calcination temperature. Correspondingly, increasing the calcination temperature promotes the catalytic oxidation of BPA. The positive correlations between the contents of pyridinic-N and graphitic-N and the kobs values of BPA oxidation, as well as XPS analysis indicate the important roles of pyridinic-N and graphitic-N in BPA oxidation. According to the series of characterizations of the oxidation products and Raman analysis of the reaction process, the moderately activated persulfate (PS) on the CN catalyst is the predominant species in BPA oxidation and BPA can be oxidized to BPA polymers with high selectivity by H-abstraction under alkaline conditions. This work highlights the important role of the moderate activation of PS in the polymerization of phenolic contaminants under alkaline conditions, which enriches our understanding of the oxidation of aromatic contaminants by PS under alkaline conditions.
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高影响因子
Nanoscale
·
2023
·Vol. 15
·期 20
·9214-9228
·
IF 6.7
Wenting Li,Shikai Liu,Yangyang Zhang,Jialing Zhou,Rumin Li,Shili Gai,Lei Zhong,Piaoping Yang
Numerous research studies have proved that lactate is pivotal in tumor proliferation, metastasis, and recurrence, so disrupting the lactate metabolism in the tumor microenvironment (TME) has become one of the effective methods of tumor treatment. Herein, we have developed a versatile nanoparticle (HCLP NP) based on hollow Prussian blue (HPB) as the functional carrier for loading α-cyano-4-hydroxycinnamate (CHC), and lactate oxidase (LOD), followed by coating with polyethylene glycol to enhance chemodynamic therapy (CDT) and the antimetastatic effect of cancer. The obtained HCLP NPs would be degraded under endogenous mild acidity within the TME to simultaneously release CHC and LOD. CHC inhibits the expression of monocarboxylate transporter 1 in tumors, thereby interrupting the uptake of lactate from the outside and alleviating tumor hypoxia by reducing lactate aerobic respiration. Meanwhile, the released LOD can catalyze the decomposition of lactate into hydrogen peroxide, further enhancing the efficacy of CDT by generating plenty of toxic reactive oxygen species through the Fenton reaction. The strong absorbance at about 800 nm endows HCLP NPs with excellent photoacoustic imaging properties. Both in vitro and in vivo studies have demonstrated that HCLP NPs can inhibit tumor growth and metastasis, providing a new possibility for tumor therapy.
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FOOD CHEMISTRY
·
2021
·
IF 7.514
Xiaomin Chen,Hui Wang,Xiaojun Huang,Shengkun Xia,Chunhua Chen,Qixing Nie,Shaoping Nie
This work established an effective method for kale flavonoids enrichment by resins. Resin screening, adsorption kinetics and isotherms, dynamic adsorption and desorption tests were conducted to optimize the appropriate resins and enrichment conditions. The results showed that NKA-9 was the optimum resin. The best adsorption conditions were 0.2 mg/mL flavonoids concentration, 12.5 bed volume (BV) sample volume and 2 BV/h adsorption rate. The desorption conditions were 3 BV of 80% ethanol at 2 BV/h elution rate. Under these conditions, the product purity was 31.16%. The purified flavonoids extract was mainly comprised of Kaempferol-3-O-sophoroside-7-O-diglucoside, Kaempferol-3,7,4′-O- d -triglucoside, Kaempferol-3-O-feruloyl-sophoroside-7-O- d -glucoside, and Kaempferol-3-O-sinapoyl-sophoroside. Moreover, it presented higher scavenging ability against 1,1-diphenyl-2-picrylhydrazyl (DPPH) radical and hydroxyl ( OH) radical than crude extract. In conclusion, kale flavonoids can be well concentrated by NKA-9 resin and the purified flavonoids extract has good antioxidant activity which can be potentially applied in food, cosmetic or pharmacy industries.
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高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Peipei Huang,Lili Yao,Qing Chang,Yunhan Sha,Guodong Jiang,Shenghua Zhang,Zhe Li
The slow redox rate of Fe(III)/Fe(II) couples is a rate-limiting step for Fenton-like performance of Fe-MOFs. In this study, a series of catalysts (MIL-101) with various p-phthalic acid/2-aminoterephthalic acid (H 2 BDC/NH 2 –H 2 BDC) molar ratios were prepared using a simple and mild chemical method and applied for catalyzed degradation of bisphenol A (BPA). Interestingly, the –NH 2 modified MIL-101(Fe) can adjust Fe-Oxo node by increasing the electron density of Fe(III) in the presence of –NH 2 group with high electron density, thus forming Fe(II) in situ in MOFs. Meanwhile, the –NH 2 groups used as electron-donors can promote electron transfer , resulting in faster Fe(III)→Fe(II) half-reaction and active H 2 O 2 to continuously generate •OH radical. The BPA degradation and rate constant of Fe-BDC-NH 2 /H 2 O 2 system are 15.4-fold and 86.8-fold higher than that of Fe-BDC/H 2 O 2 system, respectively. The density functional theory (DFT) calculations showed that Fe-BDC-NH 2 possesses higher Fermi level energy (−4.88 eV) and lower activation energy barriers (0.32 eV) compared with Fe-BDC. Moreover, Fe-BDC-NH 2 showed good reusability and stability. This work offers a highly efficient and stable MOFs-based Fenton-like catalyst to rapidly degrade organic pollutants over a wide pH range for potential applications in wastewater treatment .
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高影响因子
WATER RESEARCH
·
2021
·
IF 11.236
Chenying Zhou,Peng Zhou,Minglu Sun,Yang Liu,Heng Zhang,Zhaokun Xiong,Juan Liang,Xiaoguang Duan,Bo Lai
The sluggish kinetics of Fe(II) recovery strongly impedes the scientific progress of Fenton reaction (Fe(II)/H 2 O 2 ) towards practical application. Here, we propose a novel mechanism that metal-free nitrogen-doped carbon nanotubes (NCNT) can enhance Fenton chemistry with H 2 O 2 as electron donors by elevating the oxidation potential of Fe(III). NCNT remarkably promotes the circulation of Fe(III)/Fe(II) to produce hydroxyl radical ( • OH) with excellent stability for multiple usages (more than 10 cycles) in the NCNT/Fe(III)/H 2 O 2 system. Although carbonyl on NCNT can act as the electron supplier for Fe(III) reduction, the behavior of NCNT is distinct from common reductants such as hydroxylamine and boron. Electrochemical analysis and density functional theory calculation unveil that nitrogen sites of NCNT can weakly bind with Fe(III) to elevate the oxidation potential of Fe(III) (named near-free Fe(III), primarily FeOH 2+ ) at pH ranging from 2.0 to 4.0. Without inputs of external stimulations or electron sacrificers, near-free Fe(III) can promote H 2 O 2 induced reduction of Fe(III) to initiate Fenton chain reactions for long-lasting generation of • OH. To our delight, it is a common property of N-doped carbon materials (e.g., graphene, carbon nanofibers, and acetylene black), our research thus provides a novel, sustainable, and green strategy for promoting Fenton chemistry.
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高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Caihong Qin,Chaochao Jiang,Mengke Guo,Rongrong Liu,Rui Yu,Jiayu Huang,Dongjie Yan,Shijie Li,Xiaoqing Dang
By-product ozone emission is one of the challenges for applying dielectric barrier discharge (DBD) technology for volatile organic compounds (VOCs) removal. In this study, a DBD reactor followed by a wet scrubber (WS) containing a solution of metal ions (Fe 2+ /Mn 2+ /Cu 2+ ) was used to reuse ozone for further oxidation of typical VOC toluene. Compared with the degradation effect of the DBD reactor alone, DBD coupled WS/iron system not only improved the toluene removal efficiency but also significantly reduced the ozone emission. The ozone removal efficiency reached as high as 98% in the DBD coupled WS/Fe 2+ system. Electron paramagnetic resonance (EPR) tests showed that ozone was converted into radicals such as hydroxyl radicals in Fe 2+ and Cu 2+ solution, which further oxidized toluene in WS/iron. Quenching experiments showed that the contribution for toluene degradation by radicals was up to 75% and 62% in Fe 2+ and Mn 2+ reactor, respectively. This study demonstrates that the DBD coupled WS system has the potential to be an environmentally friendly technology for gaseous VOCs removal.
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高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Youru Yao,Xin Hu,Yong Zhang,Huan He,Shiyin Li
Ferrous sulfide (FeS) and humic acid (HA) are typical black substances in black bloom water. Based on the strong reduction ability of FeS and the photosensitivity of HA, the transformation of toxic organic pollutants by the combination of FeS and HA (HA-FeS) is not clear. In order to explore this issue, the stability of HA-FeS was analyzed by measuring the hydrodynamic diameter and zeta potential of HA-FeS, and then the removal mechanism and possible degradation pathway of tetrabromobisphenol A (TBBPA) by HA-FeS under continuous illumination were discussed. The results showed that the hydrodynamic diameter of FeS was reduced and the stability of FeS was improved, and it was easily suspended after FeS combined with the HA in the water. The combination of HA and FeS promoted the removal of TBBPA in water, no matter it was in the presence or absence of light. Besides, compared with the absence of light, the removal efficiency of TBBPA was improved by HA-FeS with continuous light. There were two reasons for the increase in the removal efficiency of TBBPA by HA-FeS. On the one hand, Fe 2+ and S 2− of HA-FeS had more stable chemical valence and obtained better reducibility under continuous light than that in the dark. On the other hand, light induced the release of active species ( O 2 − , 1 O 2 , and OH) in the HA-FeS composite colloid and further promoted the degradation of organic pollutants. Therefore, the black substances (FeS) of black blooms may play a beneficial role in the removal of pollutants under sunlight.
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高影响因子
JOURNAL OF POWER SOURCES
·
2021
·
IF 9.127
Zhengwei Zhou,Yanping Cui,Ying Huang,Jungang Cao,Ruojie Wu,Lili Liang,Zhaoqiang Huang
To conquer the challenges in conventional electro-Fenton (EF) such as catalyst deactivation and expensive modified cathode material , commercial molybdenum powder (Mo) is firstly applied as co-catalyst in GACSS (the cathode fabricated by granular active carbon wrapped with stainless steel mesh) EF process for organic contaminants degradation. The intermittent energy saving system is proved to enhance the co-catalytic performance, without external O 2 aeration, extra catalyst addition and pH adjusting. Optimal parameters are 50 mA applied current, 0.15 g/L Mo and 10 min on-10 min off power frequency in intermittent Mo-GACSS system, where 94.03% Rhodamine B (RhB) removal and 0.0467 min −1 degradation rate constant in 60 min is remarkable than other systems. Electron spin resonance (ESR) and quenching experiment confirm the major dominant radicals are superoxide radical (·O 2 − ) and singlet oxygen ( 1 O 2 ), which originate from Fe 2+ catalyzing and active site on Mo surface. Furthermore, the long-term consecutive experiments and characterization analysis are investigated to prove the stability of Mo-GACSS system. Various contaminants removal and electric energy consumption evaluation confirm the superiority of wide application and cost-effectiveness. The study combines co-catalyst Mo and low-cost GACSS to provide new perspective in practical organic wastewater treatment to reduce energy consumption.
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高影响因子
Journal of Water Process Engineering
·
2021
·
IF 5.485
Wen Huang,Yaxin Tang,Xueping Zhang,Ze Luo,Jianqiang Zhang
The pollution problem of livestock manure generated by the rapid development of farming industry is becoming more and more serious, and its conversion into functional materials through a new way is of great practical significance for its resource utilization. For the first time, nano zero-valent iron (nZVI)/biochar composites (Fe-RMC-850) were prepared by carbonizing Fe 3 O 4 -rabbit dung and used to activate PMS for degradation of sulfamethoxazole (SMX). The results showed that Fe-RMC-850 had high catalytic activity due to its rich pore, high graphitization and defective structure. When the dosage of Fe-RMC-850 and PMS were 0.3 g/L and 0.25 g/L respectively, the degradation rate of SMX could reach 100% within 20 min, and it still showed good catalytic stability after 5 cycles of experiments. The radical quenching, EPR and XPS results showed that radical and nonradical pathways acted synergistically in the degradation of SMX, in which nZVI, Fe 2+ -biochar and pyridinic N were used as the main active sites of the radical pathway. The nonradical pathway was attributed to the generation of C-O and COO by the oxygen-containing functional groups on the biochar surface. Moreover, the inherent P atoms formed P C and CPO 3 /C 2 PO 2 , thereby producing defective structures, while the graphitic carbon layer provided good electron transfer sites. Consequently, this study provides a nZVI-rabbit manure biochar composite PMS catalytic material with high organic pollutant degradation efficiency and offers a new option for the resource utilization of manure sources.
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CATALYSIS LETTERS
·
2021
·Vol. 152
·期 9
·2607-2624
·
IF 3.186
Zhang Qian,Chen Si,Yu Yong Bo,Hong Jun-ming
Simultaneous pollution degradation and disinfection were seldom discussed in the field of electrocatalytic oxidation. In this work, N-doped graphene (N-GN) was selected as anode to ensure the high performance of paracetamol (APAP) degradation. With N doping, the activity of N-GN is evidently improved because of the better surface area, active defects, and conductivity compared with graphene. The generation of active chlorine and O 2 . − on the N-GN surface played an important role in APAP degradation. Compared with other operation parameters (such as pH and current density), environmental microorganisms exhibited more negative interference for APAP degradation. However, evident disinfection effects can be observed because of the release of fulvic and humic acids from microorganisms. In particular, active chlorine is evidently more effective than O 2 . − for disinfection. The simultaneous APAP degradation and disinfection observed in this research provided the possible technology of electrocatalytic oxidation via N-GN for practical application. Graphical Abstract
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Peng Huang,Peng Zhang,Cuiping Wang,Jingchun Tang,Hongwen Sun
Persulfate-based (PS-based) advanced oxidation process is a promising technology for degradation of organic pollutants . PS activation needs efficient and economical catalysts and heterogeneous Fe-carbon composites are competitive. Herein, novel N-doped biochar-loaded nanoscale zero-valent iron (nZVI) composites (Fe@N-BC) were synthesized and evaluated for PS activation. Detailed characterization data indicated that graphitic and pyridine N structures were introduced by N-doping, which enhanced the anchoring, dispersion and loading of amorphous nZVI on biochar. Remarkably, the optimized Fe@N-BC material, Fe@N 2 -BC 900 , presented excellent catalytic performance for PS activation for lindane removal. The N-doped defects in biochar acted as reactive bridges and accelerated the electron transfer between nZVI and PS, showing strong synergistic effects toward nZVI. O 2 • − and 1 O 2 were the dominant active species in catalytic systems. Additionally, Fe@N 2 -BC 900 catalyst showed effectiveness over a wide pH range for lindane removal. This work provides a new approach to the rational design and application of Fe@N-BC for persulfate activation in pollution control, which is certified by deep exploration of reaction mechanism.
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Journal of Cleaner Production
·
2021
·
IF 9.297
Antony Rajendran,Hong-Xia Fan,Tian-You Cui,Jie Feng,Wen-Ying Li
SO x emission, one of the significant contributors to air pollution, is primarily caused by the combustion of sulfur-containing liquid fuels . Thus, ultra-low sulfur or sulfur-free fuels production gains more attention to construct the SO x -free environment. Despite the oxidative desulfurization using polyoxometalates and hydrogen peroxide showing promising results, the requirement of hydrogen peroxide in excess and the complicated synthesis of heterogeneous polyoxometalates are the key drawbacks. So, in this paper, facile hydrothermal synthesis of mesoporous tin oxide-supported octamolybdates containing Mo V and Mo VI sites is reported for oxidative desulfurization with near stoichiometric hydrogen peroxide. The current catalytic system seems competitive among molybdenum-based oxidative desulfurization catalysts due to its higher turnover frequencies of 28.1 h −1 . The straightforward synthesis of catalysts and their excellent oxidative desulfurization activity would be attractive in building the SO x -free environment via clean transport energy.
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