MATERIALS CHEMISTRY AND PHYSICS
·
2022
·
IF 4.778
Lingli Ji,Qixing Xiao,Lijun Zhu,Sridhar Komarneni,Jianfeng Ma
Carbon dots (CDs)-modified Cr 2 O 3 (CDs@Cr 2 O 3 ) composites were synthesized by solvothermal process followed by calcination to improve their catalytic performance. The physical and chemical properties of the composites were determined by XRD , SEM , TEM, BET and XPS . With the aid of sodium persulfate, the activity of CDs@Cr 2 O 3 to oxidize Orange II by non-radicals was studied under various conditions. The experimental results determined the optimal dosage of PDS to be 0.1 g and the degradation results showed that after 45 min, the degradation rate of Orange II reached to 98.4% with the CDs@Cr 2 O 3 /PDS/Vis system. The adsorption capacity of CDs@Cr 2 O 3 for Orange II was closely related to pH, and this phenomenon is further explained by the isoelectric point. A series of experiments proved that non-free radicals played a crucial role in the oxidation process , in which singlet oxygen ( 1 O 2 ), superoxide radical (O 2 •− ) and photo-generated holes (h + ) were determined as the important reactive oxygen species (ROS). In addition, the present study found that increasing dissolved oxygen could promote the reaction and the catalyst maintained good degradation performance after five cycles suggesting its stability.
✓ 已验证
产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2022
·
IF 8.634
Lincai Peng,Xin Huangfu,Yao Liu,Huai Liu,Junhua Zhang
The processing of C6 sugars to alkyl levulinate (AL), a versatile biomass-derived building block, can be readily implemented via the straightforward acid-catalyzed reaction in alcohol medium while it remains a challenge to produce AL from C5 sugars in the one-pot procedure over a monolithic catalyst. In this contribution, a budget and multifunctional natural lignocellulose welded Zr–Al bimetallic hybrid (ZrAl@CS-MSA) has been successfully constructed with crude corn stalk as a sustainable support. The becoming Lewis and Brønsted acid sites of ZrAl@CS-MSA catalyst guarantee a high AL yield of 54.3% from xylose via a one-pot process in a renewable n -butanol medium. Experimental findings revealed that the sulfonic group of ZrAl@CS-MSA plays a significant role in the xylose dehydration, furfuryl alcohol etherification and alcoholysis reactions while Zr species is in charge of the transfer hydrogenation of furfural. The Al species enclosed in ZrAl@CS-MSA can regulate its Brønsted and Lewis acidity, accelerating the etherification and alcoholysis reactions as well as alleviating the over hydrogenation of AL. This work opens a green, sustainable and reliable avenue for producing C5 sugar-based AL using natural lignocellulose-related multifunctional catalysts.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Peng Xu,Shiqi Xie,Xin Liu,Lei Wang,Xiangwen Jia,Chao Yang
CuFe 2 O 4 (CFO) nanoparticles have been used to induce peroxymonosulfate (PMS) for degrading contaminants, while the slow reduction from high valence metals to low valence metals on CFO surface limited its reaction activity. In our study, the introduction of electric field greatly enhanced the activation of PMS by CFO for the degradation of diclofenac (DCF). The removal efficiency and the electrical energy per order of the EC/PMS/CFO system reached 89.9% and 2.12 kWh m −3 order −1 respectively within 60 min under optimal conditions of 0.3 g/L CFO, 2 mM PMS, 8 mA/cm 2 current density and initial pH of 6. Electron spin resonance analysis and quenching experiments including ethanol, tertbutyl alcohol, furfuryl alcohol and p-benzoquinone proved that SO 4 •− , •OH and 1 O 2 were the main reactive oxygen species in the EC/PMS/CFO system. The cyclic voltammetry test and the X-ray photoelectron spectroscopy demonstrated that both PMS and electric field accelerated the cycles of Fe(III)/Fe(II) and Cu(II)/Cu(I), promoting the generation of reactive oxygen species. Except for the inhibition effect of humic acid and HPO 4 − , NO 3 − had no impact on the degradation of DCF, while HCO 3 − and Cl − accelerated the degradation of DCF in the EC/PMS/CFO system. Furthermore, >90% of DCF in tap water and Houhu lake water was degraded by the EC/PMS/CFO system. The reusability experiment verified that CFO was stable, and the leaching concentrations of copper and iron in each run were less than the legal limits of the U.S. Environmental Protection Agency. This work might provide a feasible strategy for enhancing PMS activation through coupling transition metals with an electric field.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yuhan Long,Songrong Li,Peizhen Yang,Xi Chen,Wenhao Liu,Xuesong Zhan,Cheng Xue,Dongfang Liu,Wenli Huang
MOF-derived metal-carbon composite catalyst was an alternative high-efficient catalyst for activating peroxymonosulfate (PMS). In this study, a novel cobalt-carbon-nitrogen doped composite catalyst with honeycomb porous structure (Co-HPNC) was obtained through a simple strategy consisting of three steps: self-growth of ZIF-67 on the SiO 2 core, pyrolysis, and NaOH etching away SiO 2 core. The Co-HPNC exhibited an outstanding catalytic performance (98.1% in 10 min) to activate PMS for acid orange 7 (AO7) degradation. The observed reaction kinetic constant (0.4319 min −1 ) was 2.64 times superior to that of the unmodified Co/NC catalysis system (0.1636 min −1 ). In the meantime, the catalyst demonstrated a high PMS activation capacity over a wide pH range of 3–11 and strong adaptability to the high concentration of inorganic anions (Cl - , SO 4 2- , and CO 3 2– ). After being recycled three times, the removal efficiency could still reach 92.7% in 25 min. The quenching tests and EPR spectrum illustrated the existence of radical and non-radical pathways, in which singlet oxygen was dominant during the degradation process. It was hypothesized that Co(0)/Co(Ⅱ)/Co(Ⅲ), pyridinic-N and pyrrolic-N contributed to the generation of hydroxyl and sulfate radicals, while C=O functional group and graphitic-N were catalytic sites for singlet oxygen. Finally, the radical electrophilic attacking sites of AO7 were calculated by the density functional theory (DFT), and the degradation routes of AO7 were speculated by GC–MS. The toxicity test illustrated that the Co-HPNC/PMS system was an environmental-friendly technology for AO7 degradation. The prepared Co-HPNC with a unique honeycomb porous structure presents a novel synthesis route for MOF-derived catalyst applied in the PMS activation system for wastewater treatment.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Zelin Wu,Zhaokun Xiong,Rui Liu,Chuanshu He,Yang Liu,Zhicheng Pan,Gang Yao,Bo Lai
Metal leaching and catalytic stability are the key issues in Fenton-like reaction. Herein, a hollow yolk-shell nanoreactor (HYSCN) with shell confined Co species was fabricated for peroxymonosulfate (PMS) activation to degrade carbamazepine (CBZ). The uniform Co nanoparticles were completely anchored in a hollow void, further confined by a porous N-doped carbon shell. The unique construction significantly reduces Co species leaching in PMS activation and enhances catalytic stability. Co leaching came from HYSCN dropped by almost fourfold compared to CN-8 without shell confined (0.403 mg/L to 0.120 mg/L). The catalytic stability is also greatly improved, confirming the dominant role of heterogeneous catalysis in the HYSCN/PMS system. HYSCN exhibits excellent catalytic performance compared to a solid structure (SCSCN), demonstrating the significance of hollow structures. Mechanism study found that HO • , SO 4 • – and 1 O 2 induced in HYSCN/PMS system and the relative contributions were distinguished and quantified by stoichiometric methods. The UPLC-Q-TOF-MS/MS was used to identify the CBZ degraded intermediate products and the possible degradation pathway was proposed. This study will provide theoretical guidance for reducing metal leaching and improving catalytic stability in the PMS activation.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yi Han,Mingjie Huang,Wei Xiang,Chen Wang,Yongjie Li,Xiaohui Wu,Juan Mao,Tao Zhou,Hong Li,Deming Wu
Fe-based metal–organic frameworks (MOFs) are popular in activating oxidants e.g·H 2 O 2 and persulfate (PS) for degrading recalcitrant organic substances, generally regarded with a simple interfacial efficient iron cycle. This study has revealed that a novel two-steps single-electron transfer mechanism would occur initially to activate the rapid degradation 4-chlorophenol (4-CP) in the MIL-88B(Fe)/H 2 O 2 system (88B/H 2 O 2 system). The degradation of 4-CP was acidic favorable (pH 0 ≤ 6.0) and could be divided into two reaction stages, i.e., initial lag phase (0–10 min) and following rapid decay phase (10–50 min). In the first stage, H 2 O 2 was slowly activated on the surface of 88B to form superoxide radical (O 2 •– ), which would lead to the accumulation of the key intermediate hydroquinone (HQ) through reducing 4-CP. Afterwards, HQ could reductively dissolve iron ions which would lead to the subsequent efficient homogeneous Fenton reaction for the rapid oxidation of 4-CP by hydroxyl radical (•OH) in the following rapid decay phase. It was interesting to note that specific aromatic compounds, which would form reductive benzenediols intermediates by O 2 •– , could be efficiently degraded in the 88B/H 2 O 2 system. The result of this study is expected to provide a new insight for understanding the catalytic oxidation process based on MOFs, and its application if possible.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xinxin Long,Chuanping Feng,Shengjiong Yang,Dahu Ding,Jinpeng Feng,Meng Liu,Yang Chen,Jihua Tan,Xingjie Peng,Jinan Shi,Rongzhi Chen
Oxygen atoms with lone pair electrons have been used to improve the photocatalytic activity of graphitic carbon nitride (g-C 3 N 4 ). Herein, a one-step annealing strategy without co precursor is used to prepare O-doped graphitic carbon nitride (OCN) for photocatalytic degradation of bisphenol A (BPA). The band structure and photocatalytic performance are tuned by simply controlling the heating time. The degradation rate constant for OCN6 is improved by 29 times compared to the original CN. Experimental and the density functional theory calculated results prove that the doped-O is the key factor in promoting photocatalytic performance. The introduced O not only adjusts local electron density, but also decreases the band gap to boost e - transfer and carrier generation and separation. The elevated conductive band energy is responsible for producing O 2 ∙ - , which is the dominated reactive oxygen species. This work offers a simple and effective way for the self-modification of metal-free catalysts to resolve environmental issues.
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Wenwei Feng,Yousef Faraj,Yuan Yan,Yaoxiao An,Ruzhen Xie,Bo Lai
The design of a high-efficiency and ecofriendly persulfate (PS) activator with low cost and superior performance in water decontamination still remains a big challenge. Herein, we report a facile strategy for the synthesis of novel pyrolusite-templated mesoporous catalyst (PMC), and used it as a green PS activator for the outstanding removal of bisphenol A (BPA) in water. The N2 adsorption–desorption curves and SEM-EDS images show that pyrolusite templating can successfully modulate the mesoporous structure of the catalyst; the XRD and XPS spectra indicate that pyrolusite templating renders the catalyst with enriched active sites and faster electron transfer. The mechanism studies suggest that both the radical and nonradical pathway [singlet oxygen (1O2)] contributed to BPA degradation, and 86.81% of the total organic carbon (TOC) of 100 mg/L BPA was removed using merely 0.4 g/L PMC, without detectable metal ion leaching. This work provides a new strategy for the structural design and property adjustment of an efficient persulfate catalyst for green environmental remediation.
✓ 已验证
产品关联
DOI
高影响因子
Environmental Science-Nano
·
2022
·Vol. 9
·期 3
·1091-1105
·
IF 9.473
Heng Shi,Yi He,Yubin Li,Teng He,Pingya Luo
Metal–organic frameworks (MOFs) for persulfate-based Fenton-like processes have attracted tremendous attention nowadays. However, the low utilization of active sites and poor stability of MOFs still impede their practical application. In this work, we demonstrate a unique photo Fenton-like catalyst with confined ultrasmall MOF nanoparticles anchored on a 3D-graphene network, which is fabricated through a simple confined thermal pulverization method. The ultrasmall Co–Fe MOF nanoparticles with confined structure endowed this catalyst with highly exposed active sites as well as excellent stability. It can maintain high degradation efficiency via visible light-assisted peroxymonosulfate (PMS) activation in a broad pH range from 1–13. Electron spin resonance (ESR) technology reveals that both radical and nonradical processes are involved in this process, and the broad pH adaptability of this system is due to the stable generation of ˙OH, SO4˙−, ˙O2−, and 1O2 under these pH conditions. This study provides new perspectives for the development of highly efficient and harsh environment-adaptive MOF-based Fenton-like catalysts.
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Yanqing Cong,Jiaxin Yi,Shengna Liang,Feng Zhang,Yi Zhang,Shi-Wen Lv
Bimetallic oxides with spinel structure show great prospects in the photocatalysis owing to many active sites. Herein, a novel 500NiCo 2 O 4 @CdS–5%Ag composite was fabricated via a feasible strategy. Interestingly, the combination with NiCo 2 O 4 could significantly enhance the absorption ability of CdS for visible light. Benefiting from the formation of heterojunction structure between NiCo 2 O 4 and CdS, the recombination of photogenerated electrons and holes was remarkably restrained. As an effective mediator, deposition of Ag could further promote the transfer of photogenerated charge carriers, thereby accelerating the reaction rate. Meanwhile, light absorption capacity of composite was also improved, owing to the surface plasmon resonance effect of metallic Ag. More importantly, 500NiCo 2 O 4 @CdS–5%Ag composite with great stability displayed an excellent performance in the photocatalytic degradation of OFX, and its highest removal efficiency was as high as 99.14%. Possible degradation pathways of OFX were given, and most of OFX could be degraded into CO 2 , H 2 O and other by-products with no toxicity. Significantly, the separation and transfer of photogenerated charge carriers followed indirect Z-scheme heterojunction mechanism. The O 2 − , OH and 1 O 2 were main active species in photocatalytic reaction system. All in all, current work inspired some new ideas for designing novel photocatalytic system in wastewater treatment .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Yanlin Zhang,Wei Chu
In this study, a Fe 3+ /g-C 3 N 4 hybrid catalyst system was proposed to activate peroxymonosulfate (PMS) for the metronidazole (MNZ) photocatalytic degradation . The two catalysts, Fe 3+ and g-C 3 N 4 , exhibited an obvious synergistic effect in the photocatalytic degradation process. When 1 mM PMS, 0.04 mM Fe 3+ and 0.05 g L −1 g-C 3 N 4 were applied, the rate constant of the Fe 3+ /g-C 3 N 4 /PMS/LED process at 0.07288 min −1 is around 3.6 to 6.8 times faster than that of Fe 3+ /PMS/LED and g-C 3 N 4 /PMS/LED processes at 0.0198 and 0.01076 min −1 , respectively. Under visible light, electron transfer from photo-activated g-C 3 N 4 to Fe 3+ , resulting in the continuous regeneration of Fe 2+ in the system, which ensures non-stopping production of radicals for MNZ degradation. UV–visible spectra were used to confirm the regeneration of Fe 2+ . In addition, EPR tests were used to identify the reactive oxygen species involved in the reaction system. Typically, the effects of various operation parameters, including the catalyst dosage, PMS dosage, initial concentration of MNZ and initial pH were examined. This work provided a new idea of promoting pollutant degradation by accelerating Fe 3+ /Fe 2+ redox through semiconductor, which could help to use the catalyst more effectively for wastewater treatment and/or chemical industries.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Jingyi Lin,He Zhao,Hongbin Cao,Yuehong Zhao,Chuncheng Chen
Photoinduced volatile organic compounds (VOCs) release from fatty alcohols at the air-water interface, has attracted considerable attention. This paper comprehensively explores the release of odorous VOCs from aqueous micropollutants under photoirradiation, especially in terms of the important role of the reactive oxygen species (ROS) in increased risk by cross-media transformation. The formation and distribution of photoinduced VOCs produced by aqueous benzyl alcohol (BzOH), a common ingredient in personal care products, were monitored in situ by online gas chromatography equipped with mass spectrometry and flame ionization detector (GC–MS/FID). The photoreaction of BzOH followed first-order kinetics with a rate constant of 0.0158/min under air. After 180 min of ultraviolet irradiation, the accumulated output of the gas-phase products benzene and benzaldehyde (BA) reached 3.8 μmol and 2.6 μmol respectively, being approximately 10 times that under nitrogen. According to electron paramagnetic resonance measurements, singlet oxygen mainly promoted the oxidation of BzOH to BA, which was an important intermediate producing benzene via photocleavage. Odorous alicyclic hydrocarbons were also generated through photorearrangement under nitrogen. On the other hand, the Henry's law constants of the main products were much lower than those of BzOH, indicating that the photoproducts would volatilize from the aqueous phase into the gas phase. The odor threshold of gas-phase products decreased to varying degrees after photoirradiation. Especially for BA, one of the main products, its odor threshold decreased 130 times compared with BzOH. This study shows that the risk of cross-media pollution could significantly increase due to the transformation of aqueous pollutants into odorous VOCs under photoirradiation and provides new insight into its risk prevention.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）