APPLIED SURFACE SCIENCE
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2021
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IF 6.707
Li Li,Zhi Huang,Yanying Liu,Ziqi Zhu,Mingjun Xu,Wenxuan Wei,Qian Zhang,Junming Hong
Novel porous Mn-Fe nanocubes (p-MnFe NCs) with abundant oxygen vacancies, which derived from Mn-Fe prussian blue analogue, were fabricated for the first time through annealing at H 2 atmosphere. Among the different molar ratios of Mn/Fe, p-Mn 1 Fe 1 NCs possessed abundant oxygen vacancies and exhibited excellent performance for peroxymonosulfate (PMS) activation to effectively degrade bisphenol A (BPA). As a result, 100% BPA (20 mg/L) degradation efficiency can be achieved within 30 min in the p-Mn 1 Fe 1 NCs/PMS system. SO 4 •− , HO•, O 2 •− and 1 O 2 were confirmed as main reactive oxygen species during catalytic reaction. The exposed Mn and Fe sites on the surface of p-Mn 1 Fe 1 NCs were the main active sites for the generation of reactive radicals. For non-radical generation pathway, the generated 1 O 2 and O 2 •− mainly originated from the reaction between dissolved oxygen and surface oxygen vacancies, and parts of 1 O 2 originated from the formation of intermediate O 2 •− . Radical and non-radical pathways were proposed in the p-Mn 1 Fe 1 NCs/PMS system for insights into the mechanisms of BPA degradation. Finally, the possible degradation pathways were proposed via ultra-performance liquid chromatography quadrupole time-of-flight mass spectrometry (UPLC-TOF-Q-MS) analysis.
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REACTIVE & FUNCTIONAL POLYMERS
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2021
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IF 3.975
Junyu Chu,Heng Wang,Yiwen Zhang,Zhengkai Li,Zhencai Zhang,Hongyan He,Qinqin Zhang,Fei Xu
The synthesis of bio-based polymers using renewable bio-monomers have received extensive research attention to meet the concept of environmental sustainability. Isosorbide (ISB) derived from biomass is commonly used in the polycarbonate industry as an alternative to bisphenol A (BPA) because it is green, non-toxic, and more widely available. Compared to BPA-based polycarbonate, isosorbide-based polycarbonate has excellent properties such as high transparency, easy coloration, and outstanding rigidity. However, the naturally low refractive index of isosorbide triggers the latter to fall outside the threshold of optical applications. In order to further improve the refractive index of isosorbide-based polycarbonate without affecting its transparency and rigidity, a copolymerization scheme of bisphenol monomers (BPs) with isosorbide is proposed in this work. A series of isosorbide–bisphenol copolycarbonates were synthesized by a melt polycondensation process using ionic liquid 1,4-(1,4-diazabicyclo[2.2.2]octane)butyl dibromide ([C 4 (DABCO) 2 ][Br] 2 ) as the catalyst. As expected, the monomer structure had significant effect on the optical property and molecular weight of the copolycarbonates, the monomer bis( p -hydroxyphenyl) ether (BPO) had better reactivity among the screened seven monomers resulting in relatively higher molecular weight. Moreover, poly(BPO- co -ISB carbonate) (POIC) using BPO as the monomer exhibited a high Abbe number (v d = 39.7), low yellowness index (YI = 0.93), and a higher refractive index (n d = 1.536), which was much higher than poly(isosorbide carbonate) (1.496). Therefore, a series of POICs were further prepared to investigate the effect of BPO content on the optical, thermal, mechanical, and hydrophobic properties of the materials. The results showed that the copolymers POICs had higher refractive indices (1.511–1.573), better thermal stability, flexibility, hydrophobicity and processing-friendly glass transition temperature (T g ) and pencil hardness, and thus are expected to be sustainable materials for optical lenses.
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Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Xia Zhang,Xitong Yang,Bing Liu,Guifen Zhu,Jing Fan
An approach of simultaneous iodine doping and heterojunction fabricating with basic bismuth salt was proposed, Based on this, a novel I/BiOIO 3 /[Bi 6 O 6 (OH) 3 ](NO 3 ) 3 ∙1.5H 2 O (I/BiOIO 3 /BHN) photocatalyst was prepared. The photocatalytic activity was evaluated by the degradation of multiple refractory pollutants (rhodamine B, methyl orange, phenol , bisphenol A, bisphenol B, bisphenol Z) in water under solar light irradiation. Compared with single photocatalyst, the optimized sample displayed the reaction rate constant of 0.1606 min −1 , which was 69.8, 11.4 and 2.2 times of individual [Bi 6 O 6 (OH) 3 ](NO 3 ) 3 ∙1.5H 2 O, BiOI and BiOIO 3 , respectively. The performance improvement was attributed to the inhibition of charge carrier recombination by type II heterojunction formation and the expanded solar capture range caused by the springboard effect of iodine impurity level. The photocatalytic mechanism of I/BiOIO 3 /BHN was hole oxidation , followed by·OH oxidation. Besides, the I/BiOIO 3 /BHN photocatalyst in bulk structure with micrometer size and high-density could be easily separated and recovered by simple sedimentation, confirming its good application prospect in the wastewater treatment .
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Huiwang Dai,Wenjun Zhou,Wei Wang,Zhiqi Liu
In this study, three Co/N-C catalysts were prepared by pyrolysis of bimetallic zeolitic imidazole frameworks with different Co/Zn ratio, and the critical active Co species in peroxymonosulfate (PMS) activation was investigated. The three catalysts had distinct cobalt species but similar N configuration and graphitization degree. The Co species were distributed as single atoms (Co SAs) at a Co/Zn molar ratio of 1:8, while Co nanoclusters (Co NCs) and Co nanoparticles (NPs) would be formed with further increase in Co content. The degradation efficiency of BPA did not show correlation with the increasing of Co content in catalyst. Based on the catalytic performance comparison and reactive species detection, Co SAs was identified as active sites, which could interact with PMS to generate 1 O 2 via path of PMS→HOO*→O*→ 1 O 2 . However, the role of NCs and NPs in directly activating PMS was negligible. In addition, the increase of Co content in Co/N-C catalyst would result in mass cobalt leaching, which enhanced the BPA degradation via homogeneous catalytic reactions with Co IV as reactive species. It is an effective way to design the Co/N-C catalyst with high catalytic activity and stability via regulating the formation of Co SAs.
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高影响因子
WATER RESEARCH
·
2021
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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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JOURNAL OF HAZARDOUS MATERIALS
·
2021
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IF 10.588
Yantao Wan,Wei Zhang,Xiaolin Han,Lei Zhou,Huajun Zhen,Chengzi Wu,Qi Yu,Guangli Xiu
A novel B,N-decorated carbocatalyst (Fe@BPC-XBN) for peroxymonosulfate (PMS) activation was prepared by a simple pyrolysis method using the iron-based metal organic frameworks (Fe-MOF), boric acid and boron nitride (BN) as precursors. Fe@BPC-20BN removed 93.3% of bisphenol A (BPA) in 90 min compared to 64.9%, 82.1% and 83.5% with Fe@PC, Fe@BPC and Fe@PC-20BN, respectively, with 0.15 g/L catalyst and 1 mM PMS at initial pH of 7. The solo B-doping with boron acid on the Fe-MOF derived porous carbon enhanced its catalytic capacity; moreover, B, N co-doping with BN and boron acid as precursors further promoted the catalytic performance. The addition of BN not only provided more B, N catalytic centers but also improved the stability of the carbocatalyst. In addition, hydroxyl radicals , sulfate radicals, superoxide radicals, and singlet oxygen species were involved in the degradation of BPA. Fe species, –BCO 2 /–BC 2 O, pyridinic N, and pyrrolic N groups on the carbon matrix played the important roles in the BPA degradation. The outstanding catalytic performance of Fe@BPC-20BN could be attributed to the synergistic effects between iron nanoparticles and the B/N codoped carbon matrix. This study gives new insights into the design and preparation of high-efficient B,N-decorated carbocatalysts for environmental remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Ying Lu,Fujian Yang,Siyuan Chen,Wenchao Shi,Chengdu Qi,Guilong Peng
In this work, Ni(II) was used as peroxymonosulfate (PMS) activator for decomplexation of Ni(II)-citrate, and subsequently applied for the decomplexation of chelated nickel in the electroless nickel plating wastewater. Effect of the co-existed substances (HCO 3 − , HPO 3 2− , H 2 PO 2 − , and P 2 O 7 4− ) on the decomplexation of Ni(II)-citrate were evaluated. Interestingly, except for H 2 PO 2 − , the presence of HCO 3 − , HPO 3 2− , and P 2 O 7 4− enhanced the decomplexation efficiency of Ni(II)-citrate via promoting the decomposition of PMS. Based on the radical quenching experiments and electron spinning resonance (ESR) spectra analysis, OH, SO 4 ‐ , and 1 O 2 were the primary reactive species involved in the decomplexation reaction process. Furthermore, after the decomplexation of the electroless nickel plating wastewater by PMS, the recovery of nickel was successfully achieved via adsorption coupled with electrodeposition , and 93.1% nickel recovery could be accomplished with initial Ni(II) eluent concentration of 32.5 g/L. Therefore, this study provides a green and promising approach for the application of advanced oxidation processes based on PMS activation, and has the potential to convert recoverable resources into value-added products from electroplating wastewater.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Biao Ma,Bin Li,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Yuanzhi Zhu,Wenchao Peng
In this study, a facile atmospheric pressure chemical vapor deposition (CVD) method is used for the synthesis of nitrogen and sulfur co-doped hollow carbon sphere (NSC). Nano-CaCO 3 is used as template for the formation of hollow and highly hierarchical porous carbon structure. The doped percentages of N and S can be easily regulated by changing the ratio of N and S precursors and the deposition temperature. The obtained NSC is highly active for the catalytic oxidation of organic pollutants with peroxymonosulfate (PMS) as oxidant, and the reaction rate constant is 4.5 and 32.7 times faster than the single N or S doped samples, respectively. The PMS activation mechanism is comprehensively investigated by electron paramagnetic resonance (EPR) and radical quenching tests. Superoxide intermediate (O 2 •− ) and singlet oxygen ( 1 O 2 ) play the dominant role for phenol degradation. Moreover, with the introduction of secondary doped S atoms, more O 2 •− are generated for organics degradation. The excellent catalytic activity of NSC should be resulted from the optimized N and S doping percentages and large specific surface area (SSA). The synthesis strategy in this study provides a facile and low-cost synthetic method for heteroatom doped carbon materials and would expand the application of metal-free materials in the environmental remediation field.
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ACS ES&T Engineering
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2021
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IF 0
Zihao Zhao,Xinhong Li,Hongchao Li,Jieshu Qian,Bingcai Pan
The combination of Co(II) and peracetic acid (PAA) is an important alternative advanced oxidation process (AOPs), in which R-O• radicals including acetyloxyl radicals (CH3C(O)O•) and acetylperoxyl radicals (CH3C(O)OO•) have been considered to be the primary reactive species for the oxidative degradation of contaminants. However, it is still unclear how the active Co species participates in this process. In this study, we conduct a series of experiments including chemical probing, radical quenching, electron paramagnetic resonance (EPR), and Co(III) oxidation to investigate the degradation mechanism of contaminants in the Co(II)/PAA process, using bisphenol A (BPA) as target pollutant. On the basis of these results, we propose a Co(II)-PAA complex (Co(II)-OO(O)CCH3) to be the primary reactive species, while R-O• radicals and Co(III) (available as dimeric Co-peroxide species) derived from the decomposition of Co(II)-PAA complex are the minor contributors for the oxidation of BPA. Factors, including PAA concentration, Co(II) concentration, solution pH, inorganic anions, and natural organic matters (NOM), that might affect the oxidation performance of the Co(II)/PAA process were also investigated systematically. This study sheds new light on the mechanistic understanding of the Co(II)/PAA process for the oxidation of contaminants in water.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2021
·Vol. 29
·期 4
·6360-6374
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IF 4.223
Wu Jiawei,Xie Haijian,Zhang Chunhua,Bouazza Abdelmalek,Sun Zhilin,Qiu Zhanhong
The leakage of chemical compounds in landfill leachate led to serious environment pollution, especially, the compounds termed endocrine disruptors such as bisphenol A (BPA). It is very important to study the adsorption behavior of endocrine disruptors in modified soil for predicting and evaluating the potential harm of endocrine disruptors to the soil. Bentonite-amended Chinese loess mixtures, with various proportions of bentonite, were used for the removal of BPA from an aqueous solution. A batch test was used to investigate the adsorption properties of bisphenol A on bentonite and Chinese loess mixtures. The influences of bentonite proportion, temperature, reaction time, pH, and soil-water ratios on the adsorption process were considered. The Fourier transform infrared spectra (FTIR) was used to clarify the change of functional groups before and after the adsorption of BPA on soil. The adsorption mechanism of BPA on soil was discussed preliminary. The results show that the addition of bentonite to the loess can improve the adsorption rate of BPA. The adsorption of BPA was mainly a spontaneous, exothermic, entropy decreasing physical adsorption process. The interaction between bentonite content and reaction concentration had a beneficial effect on BPA adsorption. The linear relationship between bentonite content and adsorption capacity was obtained. The results indicate that bentonite amended loess can provide a good liner for BPA.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Chao Gao,Yan-Hua Zeng,Cheng-Yong Li,Ling Li,Zhong-Hua Cai,Jin Zhou
Microbial degradation is an effective approach for the removal of Bisphenol A (BPA). During the biodegradation process, quorum sensing (QS) is a phenomenon that enables bacteria to coordinate collective behaviors based on cell density-dependent chemical signals. However, whether the degradation of BPA can be facilitated by this QS system (such as acyl-homoserine lactone, AHL) is unclear. To answer this question, the bifunctional Sphingonomas sp. strain YK5 that had BPA-degrading and AHL-producing properties was used. Biochemical analysis revealed that this bacterial strain mainly produced C8-HSL signals. Gene knockout experiments indicated that the AHL-system ( LuxI1/LuxI2 ) was required for efficient BPA degradation. RT-PCR analyses revealed that the AHL system positively regulated the relative expression of genes ( bisdA , CYP450 , hapA , ligAB , and proB ) involved in BPA degradation. Given that AHL signaling may be a common trait among BPA-degrading microorganisms and AHL system can regulate the degradation activity, manipulation of this system may be a valuable strategy to control BPA biodegradation.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Yang Zong,Hua Zhang,Yufei Shao,Wenjie Ji,Yunqiao Zeng,Longqian Xu,Deli Wu
Periodate (PI)-based advanced oxidation processes have recently received increasing attentions. Herein, PI was readily activated by nano zero-valent iron (nZVI) and subsequently led to the enhanced oxidation of organic contaminants , with the removal performance of sulfadiazine (SDZ) in the nZVI/PI process even higher than that in the nZVI/peroxydisulfate process under identical conditions. Kinetic experiments indicated that the decay of SDZ was susceptible to the dosage of nZVI and PI, but was barely affected by pH values (4.0–7.0) under buffered conditions, suggesting the promising performance of the nZVI/PI process in a relatively wide pH range. Selective degradation of contaminants and 18 O-isotope labeling assays collectively demonstrated that iodate radical ( • IO 3 ), high-valent iron-oxo species (Fe(IV)) and hydroxyl radical ( • OH) were responsible for the abatement of organic contaminants . More importantly, due to the relatively weak steric hindrance effect of PI, PI easily adsorbed on the surface of nZVI and no iron leaching was detected throughout the reaction, implying that PI activation induced by nZVI was a surface-mediated process. Besides, PI was not transformed into harmful reactive iodine species. This study proposed an environmental-friendly approach for PI activation and shed new lights on the PI-based processes.
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