APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Chuangjian Su,Ruhong Li,Chaolin Li,Wenhui Wang
The application of promising persulfate-based advanced oxidation processes (AOPs) for environment remediation is limited by the poor charge separation and the sluggish kinetic for active centers regeneration of the catalysts. Piezocatalytic activation has been proposed to solve the above concern recently, but little is known on its mechanism. Herein, novel piezocatalyst Bi 2 Fe 4 O 9 nanosheets (BFO NSs) are demonstrated to significantly improve peroxydisulfate (PDS) activation efficiency via piezocatalysis, resulting SO 4 •− and •OH as the dominant active species for organic pollutants degradation. Further DFT calculations and experimental investigations confirm that the Fe 2+ in BFO NSs as active sites donate electrons for PDS to generate SO 4 •− , and simultaneously that the piezo-electrons can accelerate the regeneration of Fe 2+ , thus leading to the superior catalytic activity. This work provides atomic-scale insights of catalytic sites and mechanisms of piezocatalytic PDS activation and may inspire the development of more efficient piezocatalysts and AOPs.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yuanxi Huang,Lingjun Bu,Yangtao Wu,Shumin Zhu,Shiqing Zhou,Zhou Shi,Dionysios D. Dionysiou
UV/sodium percarbonate (UV/SPC) advanced oxidation process is an efficient and green technology to remove contaminants of emerging concern (CECs), with the simultaneous formation of hydroxyl radical ( • OH) and carbonate radical (CO 3 •− ). This study investigated the degradation of eight CECs in UV/SPC process, including phenol, atrazine, bisphenol A, ibuprofen, sulfadiazine, acetaminophen, carbamazepine, and diuron. A model was established to simulate the experimental results, which shows that both • OH and CO 3 •− played crucial roles in UV/SPC process, and the steady-state concentrations of CO 3 •− were much higher than that of • OH. The higher concentration compensates for the low reactivity of CO 3 •− with CECs and the loss of • OH depleting by CO 3 •− . Also, the Hammett constants decreased linearly with increasing natural logarithms of rate constants, indicating the selectivity of CO 3 •− with electron-donating substituents. In real water, CEC degradation was significantly inhibited due to the competition for light absorption from background compounds and scavenging of free radicals, especially CO 3 •− , by water matrix. Further, demethylation, decarbonylation, hydroxylation, amino oxidation, and quinonization were proposed as the main reactions for CEC degradation in UV/SPC process. The minimum electrical energy per order (EE/O) was calculated as 0.152 kWh m −3 , with SPC dose of 0.138 mM and UV intensity of 2.02 × 10 -7 Einstein L −1 s −1 .
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Solar RRL
·
2022
·Vol. 6
·期 8
·2200279
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IF 9.173
Jie Deng,Wanying Lei,Junwei Fu,Huile Jin,Quanlong Xu,Shun Wang
Herein, photocatalytic selective oxidation of hydrocarbons through O 2 represents a promising way for fine chemical industry on account of its mild reaction condition. In this work, Co 3 O 4 -modified BiOBr/AgBr S-scheme heterojunction can effectively oxidize sp 3 C H bonds at benzylic position to its corresponding aldehydes, with a toluene to benzaldehyde selectivity of 94%, which is much higher than that of pure BiOBr (21.7%) and AgBr (58.9%). A unique S-scheme charge-transfer mode is confirmed for the ternary composites by the X-ray photoelectron spectroscopy and reactive species quenching measurement. The remaining photogenerated electrons in AgBr with powerful reduction ability can react with O 2 to generate •O 2 − species, which can further oxidize the benzyl radical formed on the Co 3 O 4 surface to peroxyl radicals and then thermodynamically decompose to benzaldehyde. Herein, this work has important guiding significance for the structure regulation of photocatalysts and application in selective oxidation of sp 3 C H bond of hydrocarbons.
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MICROCHEMICAL JOURNAL
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2022
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IF 5.304
Siqi Zhuang,Jianhui Jia,Ying Lin,Yi He,Yu Liu,Hui Huang,Jian-Bo Chen
The analysis of N -oxide based explosives is beneficial to avoiding explosive risk and toxic hazard to the public. Nowadays, multifunctional sensors are scarce for green extraction and analysis of N -oxide based explosives. Herein, we have designed and developed two-in-one sensing solvents (DSMs) based on deep eutectic solvents with dual functions of both extraction and detection toward N -oxide based explosives. Besides, as an extraction solvent, DSM-3 based choline chloride and urea also can detect N -oxide based explosives via color change from yellow to red. The sensing mechanism of DSM-3 toward 2,6-diamino-3,5-dinitropyrazine-1-oxide (LLM-105) as a prototype of N -oxide-based explosives has been fully investigated by experimental analysis and theoretical calculations. The proposed mechanism is based on the formation of H-bonding complexes between urea of DSM-3 and N -oxide group of LLM-105, which induces the charge transfer from urea to LLM-105. Further, this assay exhibits high selectivity, sensitivity and good visualization for the determination of LLM-105. Therefore, our study provides novel two-in-one sensing solvent for green, convenient and on-site detection of N -oxide based explosives.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Jun Wang,Ying Zhao,Chunting Li,Zijun Yu,Yang Zhang,Yuan Li,Xiaoyao Tan,Shaomin Liu,Shaobin Wang,Xiaoguang Duan
Hierarchically porous iron/nitrogen-doped carbons (Fe-N-PC) were developed for the oxidation of ibuprofen (IBP) with peroxymonosulfate (PMS). The incorporation of trace-level iron and nitrogen dopants promoted the catalytic performance remarkably, leading to 4.8, 16.4 and 22.9-fold enhancement over N-doped carbon (N-PC), porous carbon (PC), and Fe-doped carbon (Fe-PC), respectively. Fe(III) was anchored in nitrogen-coordinated pots (Fe-N x ) in the sp 2 -hybridized carbon network, and graphitic-N could synergistically boost the catalysis. Notably, methyl phenyl sulfoxide (PMSO) transformation, quenching tests, in situ electrochemical analysis and Raman spectroscopy verified high-valent iron-oxo species and direct electron transfer pathway accounted for pollutant oxidation. The relationship between the kinetic constants (ln k obs ) and the oxidation peak potential ( E op ) of pollutants was established with good correlation, manifesting particular selectivity toward oxidizing electron-rich pollutants and great immunity to background inorganic ions and natural organic matters (NOMs) for real wastewater treatment . The deactivation mechanisms of Fe-N-PC were revealed via surface oxidation and dopant refabrication. This work delicates to deepen the understanding of the nonradical mechanisms and structure-oriented PMS activation by engineered carbonaceous materials .
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PubMed
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Xiurong Zhu,Lei Ge,Wei Yan,Shengjiong Yang,Gen Wang,Delu Miao,Pengkang Jin
Heterogeneous activation of peroxymonosulfate (PMS) has been frequently proposed for the degradation of organic pollutants via the generation of reactive oxygen species (ROS). Spinel ferrite such as CoFe 2 O 4 shows great advantage for PMS activation but suffers from aggregation problem and lack of microstructure. Herein, network-like CoFe 2 O 4 immobilized on volcanic rock was synthesized for PMS activation for degrading sulfamethoxazole (SMX). The immobilized CoFe 2 O 4 network exhibited good catalytic performance for SMX removal. Systematic investigations, including in situ ATR-FTIR and Raman spectroscopy analysis, chemical quenching experiments and electron paramagnetic resonance (EPR) tests, revealed that a redox cycle of Co 2+ /Co 3+ induced the generation of ROS (SO 4 •− , OH • and 1 O 2 ) that participated in the degradation of SMX. Background constituents (e.g., inorganic ions and natural organic matters) exhibited limited influence on SMX removal. A continuous flow-through reaction in a fixed-bed column revealed the immobilized CoFe 2 O 4 network could efficient degrade SMX with long-term durability, which therefore can be a promising catalyst for PMS activation for the degradation of SMX.
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CATALYSIS TODAY
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2022
·
IF 6.562
Jinshu Huang,Yumei Jian,Hu Li,Zhen Fang
Biochar materials have wide applications in soil improvement/remediation, water pollution control, gas storage, and heterogeneous catalysis, while usually suffering from low surface areas and harsh preparation conditions. In this study, a green, environmentally friendly, and low-cost biochar catalyst (PAP-MEPP-C) was prepared by thermochemical treatment of lignin-derived monomers at a low temperature (80 °C), and further developed for high-efficiency production of biodiesel from non-edible Jatropha oil ( J O). The characterization results showed that the structure of the PAP-MEPP-C biochar catalyst was layered and 3D structure, and its acidity could be controlled by changing the monomeric composition. The reaction conditions of preparing biodiesel catalyzed by PAP-MEPP-C were optimized by the response surface method, and the obtained maximum biodiesel yield was 97.2%. The kinetics of the (trans)esterification reaction over the developed biochar catalyst PAP-MEPP-C was studied, and its superior catalytic performance to other tested acid catalysts could be supported by a relatively lower activation energy (36 kJ mol −1 ). In addition, the biochar catalyst was highly stable and could be recycled four times with more than 90% biodiesel yield.
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Colloid and Interface Science Communications
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2022
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IF 5.633
Yong-Hong Gao,Kuo Zhang,Meng-Ru Ding,Xue-Feng Gong,Hui Cao,Lei Wang
Binding-induced fibrillogenesis (BIF) peptides have a promising future in biomedicine due to the processiblity in situ in vivo, which bind to a specific trigger and in situ self-assemble into nanofibrous structures (BIF process) with excellent physical/biological functions. Alkyl chains in BIF peptides as hydrophobic tails have an important effect on self-assembly behaviors of BIF peptides. Herein, BIF peptides (trigger: Ca 2+ or integrin) with different hydrophobic alkyl chains are designed to explore the influence of hydrophobicity on self-assembly behaviors of BIF peptides (Abbreviation as BIF 4 , BIF 8 , and BIF 16 for 4, 8, 16 carbons of alkyl chains). It is found that BIF peptides with weak hydrophobicity (BIF 4 ) do not form fibrous structure upon binding to Ca 2+ , but in nanoparticle formulation. While with strong hydrophobicity, BIF 16 initially self-assemble into nanoparticles, which further bind to Ca 2+ and self-assemble into nanofibers with a β-sheet conformation. As a result, when incubated with HUVECs overexpressing integrins on surfaces, BIF 4 were internalized as nanoparticles without BIF process, but BIF 16 performed BIF process and attached on cell surfaces. This study provides experimental evidences of the hydrophobicity effect on self-assembly behavior of BIF peptides and directs applications of BIF peptides with controllable self-assembly
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JOURNAL OF APPLIED POLYMER SCIENCE
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2022
·Vol. 139
·期 29
·e52627
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IF 3.057
Xiaoqin Zhang,Jinggang Wang,Yunxiao Dong,Qianfeng Wang,Jin Zhu
The new self-healing and biodegradable copolyesters, poly(ethylene-co-diethylene glycol adipate-co-furanoate) (PEAF), were synthesized from 2,5-furandicarboxylic acid, dimethyl adipate, diethylene glycol and ethylene glycol by transesterification and polycondensation. Their number average molecular weight ( M n ) varied from 49,400 g/mol to 71,500 g/mol while the polydispersity index ranged from 1.47 to 1.97. The study showed that by adjusting the proportion of adipate segments from 25 mol% to 65 mol%, the tensile modulus was found to be ranging from 4.95 to 0.29 MPa at room temperature, which was close to or even lower than the modulus of human skin. The excellent biodegradability of PEAFs was certified by the weight loss of 34.5% to 80.9% during enzymatic degradation. Finally, self-healing properties were also discovered in PEAFs and the fastest self-healing rate observed was 23.1 μm/h for PEAF-65 at 37 °C. Due to these outstanding properties, PEAFs absolutely possess the potential to be used as human soft tissues, electronic skin, human-machine interface and so on.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Liang Zhu,Xuecui Mei,Zhengchun Peng,Jiao Yang,Yingchun Li
Paper-based microfluidic analytical devices (μPADs) have recently attracted attention as a rapid test kit owing to their low cost and nonrequirement for external driving pump. However, low accuracy and poor anti-interference ability of μPADs under complex detection condition limit their practical applications. Here, we present a facile way to prepare a novel fluorescence sensor-array μPAD for multi-analyte discrimination based on molecular imprinting technology , and its sensing behavior was studied by using three nitrophenol (NP) isomers (2-, 3-, and 4-NP) as the testing models. Carbon quantum dots (CQDs) emitting blue light were grafted on glass-fiber paper, followed by in-situ modification of three types of molecularly imprinted polymers (MIPs) with 2-, 3-, and 4-NP as template. Each sensing unit on the array showed differential yet cross-reactive binding affinity to NP isomers, resulting in distinct fluorescence quenching efficiency. Thus, precise distinguishment of the three NPs was realized with the MIPs/CQDs/paper-based sensor array. Furthermore, the discrimination ability of the platform was evaluated in mixtures of the NP isomers. Practicability of this apparatus was validated by identification of blind samples and 100% accuracy was achieved. The μPAD has proven to be highly sensitive and accurate, which will serve as an ideal analytical tool in the fields of environment monitoring, disease prognosis, food safety and so on.
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PubMed
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ANALYTICAL LETTERS
·
2022
·
IF 2.267
Caifen Chen,Dan Li,Baokang Jin
A selective, sensitive electrochemical biosensor is reported to determine bisphenol A (2,2-bis(4-hydroxyphenyl) propane, BPA) based on target-induced chain release. A gold electrode was premodified with dendritic gold nanoparticles (AuNPs) by direct electrochemical deposition to increase the active surface area of the electrode to immobilize hydrosulfonyl group-containing capture DNA (C-DNA). C-DNA was hybridized with a BPA-specific aptamer (T-DNA) to form a double helical structure. After the embedding of methylene blue (MB), this structure emitted measurable electrochemical signals. BPA specifically binds to T-DNA to form a stable BPA G-tetrad structure, thereby inducing the release of the aptamer chain and the embedded MB from the surface into solution, resulting in the reduction of the current signal. The constructed electrochemical biosensor provided a linear response to BPA concentration from 1.0 × 10−9 M to 5.0 × 10−7 M with a detection limit of 9.8 × 10−10 M. This strategy also provided good selectivity for BPA compared to similar interferents.
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POLYMER
·
2022
·
IF 4.432
Qisong Lin,Feng Gao,Yongjun Wang,Wangyang Lu,Wenxing Chen
Antimony-free poly(ethylene terephthalate) (PET) has been synthesized through polycondensation of p -phthalic acid and ethylene glycol , and then subjected to a viscosity-increasing process by liquid-state polycondensation (LSP). For both of these processes, a novel environmentally benign ethylene glycol-soluble Ti/Mg bimetal (TM) catalyst has been used. The structure of the TM catalyst has been comprehensively characterized and its catalytic activity in the polycondensation reaction has been evaluated and compared with those of other titanium-based catalysts. The results reveal that the TM catalyst is a chelated complex with high catalytic activity for polycondensation to afford PET without significant side reactions. Indeed, the LSP process catalyzed by TM affords a PET product with high intrinsic viscosity suitable for industrial yarn production (1.08 dL/g) within 60 min, and that exhibits higher thermostability with increasing intrinsic viscosity. Finally, the kinetics of the TM-catalyzed polycondensation has been probed based on the variation of intrinsic viscosity with increasing polycondensation time.
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危险品化学品经营许可证（带存储）