ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Zhuoyue Wang,Ji Li,Wei Song,Jingxin Yang,Wenyi Dong,Xiaolei Zhang
Recently, it has been reported that chlorine dioxide (ClO 2 ) and (bi)sulfite/ClO 2 showed excellent performance in micropollutant removal from water; however, the degradation mechanisms and application boundaries of the two system have not been identified. In this study, bisphenol A (BPA) was chosen as the target contaminant to give multiple comparisons of ClO 2 and S(IV)/ClO 2 process regarding the degradation performance of contaminant, generation of reactive species, transformation of products and toxicity variation. Both ClO 2 and S(IV)/ClO 2 can degrade BPA within 3 min. The BPA degradation mechanism was mainly based on direct oxidation in ClO 2 process while it was attributed to radicals (especially SO 4 · - ) generation in S(IV)/ClO 2 process. Meanwhile, the effect of pH and coexisting substances (Cl − , Br − , HCO 3 − and HA) were evaluated. It was found that ClO 2 preferred the neutral and alkaline condition and S(IV)/ClO 2 preferred the acidic condition for BPA degradation. An unexpected speed-up of BPA degradation was observed in ClO 2 process in the presence of Br − , HCO 3 − and HA . In addition, the intermediate products in BPA degradation were identified. Three exclusive products were found in ClO 2 process, in which p-benzoquinone was considered to be the reason of the acute toxicity increase in ClO 2 process.
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PubMed
高影响因子
PARTICLE & PARTICLE SYSTEMS CHARACTERIZATION
·
2023
·
IF 2.7
Yue-Feng Tang,Meng-Yun Zhao,Guo-Zhi Han
Herein, a novel composite of g-C 3 N 4 and silver nanoparticles(g-C 3 N 4 @Ag) with enhanced bifunctional catalytic activity through chemical etching is reported. A kind of g-C 3 N 4 @Ag composite by one-pot route, then treated the product with sodium borohydride (NaBH 4 ) solution for a certain time is first synthesized. The property and morphology of the g-C 3 N 4 @Ag composite changed greatly after the treatment. Compared with the pristine g-C 3 N 4 @Ag composite, the NaBH 4 -etching endowed g-C 3 N 4 @Ag composite (RACN) with smoother two-dimensional plane structure, as well as an extension of the conjugate system which originating from the stronger chemical connection between the Ag nanoparticles and g-C 3 N 4 . Furthermore, research results indicated that the RACN showed superior broad-spectrum catalytic performance for the reduction of aromatic nitro compounds, and the catalytic efficiency of the RACN is enhanced dozens of times by the treatment. Moreover, the photocatalytic activity of the RACN is also greatly improved. This discovery provides an efficient and facile method toward the enhancement of catalytic activity of semiconductor and metal nanoparticle composites by chemical etching.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yuanxi Huang,Lu Luo,Shumin Zhu,Kai Yin,Lingjun Bu,Shiqing Zhou
Peracetic acid (PAA) is a promising peroxyacid to combine with ultraviolet (UV) to eliminate trace amounts of organic contaminants (TrOCs), with growing importance in water treatment. In spite of a large number of research on UV/PAA process, the underlying mechanism still require further investigation, due to the difficulties in analyzing the carbon-centered radicals. Here we demonstrated the crucial roles of the carbon-centered radicals (namely CH 3 C(O)OO ), via electron paramagnetic resonance (EPR) and kinetic models, with concentration of 4 orders magnitude higher than that of OH. Then, the theoretical calculation using density functional theory (DFT) showed that CH 3 C(O)OO and OH tended to attack phenol mostly through the route of radical adduct formation. The generated CH 3 C(O)OO and OH adducts may undergo further reactions to produce catechol and hydroquinone. Further, the environmental applicability of UV/PAA process for TrOC abatement was evaluated, including the effects of pH, PAA dosage, water constituents, as well as the variation of acute toxicity. Different from the OH-dominated process, kinetic analysis revealed that CH 3 C(O)OO was almost immune to the presence of water constituents, leading to the outperformance of UV/PAA process in actual water samples. Our present study could inform the application of UV/PAA process in water and wastewater treatment.
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ACS Catalysis
·
2023
·
IF 12.9
Meilin Yin,LiPeng Wang,Shaokun Tang
Covalent organic frameworks (COFs) are a class of promising porous crystalline materials for both capturing and converting CO2 into high-value-added products. However, long synthesis time and the need for cocatalyst restrict its potential for CO2 conversion. Herein, bipyridine-based TAPT-BP-COF with high crystallinity as a skeleton is rapidly synthesized within only 1 h by the aid of supercritical CO2 (scCO2) activation. Then, the production of dicationic TAPT-BP2+-COF is accomplished by a quaternization reaction. The CO2 capture capacity of TAPT-BP2+-COF improved by 55.6% due to its CO2-philic groups (imine and triazine groups), polar groups (−OH), charged skeleton, and suitable pore size, thus ensuring sufficient CO2 around the catalytic active sites. Additionally, the outstanding structure-enhanced CO2 conversion performance is observed due to the presence of the synergistic effect between –OH and Br– in the TAPT-BP2+-COF skeleton. The rate-determining step of cycloaddition is significantly accelerated without any solvents and cocatalysts compared to individual TAPT-BP-COF and [OH-BP]2+[Br]2– (BP2+ moiety). Specifically, TAPT-BP2+-COF efficiently generates cyclic carbonate by heterogeneously catalyzing CO2-epoxide cycloaddition with the yield of 99.3% and has excellent stability that can be reused ten times without significant activity reduction. This work provides a novel perspective for the targeted design and rapid synthesis of charged dicationic COF-based catalysts for high efficiency and durability in CO2 capture and conversion.
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Water
·
2023
·Vol. 16
·期 1
·121
·
IF 3.4
Xiaoze Yin,Huaqin Yin,Renjie Wang,Jinnan Wang,Aimin Li
Novel Fenton-like catalyst HKUST-1(Cu)/MoS2-3-C with a non-equilibrium-state surface was constructed for selective degradation of phenolic contaminants. Electron-polarized distribution facilitated the formation of σ-Cu-ligand between electron-poor Cu centre and phenolic compounds, which not only enhanced radicals generation but also accelerated the Cu(I)/Cu(II) redox. Meanwhile, ≡Mo–OOSO3−complexes formed by the electron-rich Mo centre and peroxymonosulfate (PMS), could directly oxidize phenolic contaminants with the generation of SO4•−. The radical quenching experiments and EPR tests indicated that both SO4•−and•OH played a dominant role in the reaction. Additionally, O2could be reduced to O2•−by OVs and subsequently converted into1O2over the Mo centre. DFT calculation, FT-IR, and in situ Raman spectra analysis results demonstrated that phenolic compounds and PMS were respectively adsorbed by electron-poor Cu centre and electron-rich Mo centre, favouring the electrons transfer from phenolic contaminants to Mo centre for PMS activation. With synergistic effects of σ-Cu-ligand and ≡Mo–OOSO3−complexes, HKUST-1(Cu)/MoS2-3-C achieved a high degradation rate of phenolic contaminants and utilization efficiency of PMS.Keywords:fenton-like catalyst;non-equilibrium-state surface;σ-Cu-ligand;≡Mo–OOSO3−complex;phenolic contaminants degradation
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Bei Ye,Ziye Liu,Xiaoqin Zhu,Hanjing Wu,Zifan Liang,Wenlong Wang,Qianyuan Wu,Hongying Hu,Xinhao Zhang
Chlorination is widely used for disinfection of water and wastewater. Ammonia/chlorine co-exposure can be easily achieved when ammonia is present in water. In this study, ammonia and chlorine showed synergistic effect on atrazine (ATZ) degradation. A degradation efficiency of 50.2% was obtained in 10 min with a Cl/N molar ratio of 1.6. By contrast, free chlorine and chloramines barely degraded ATZ. The synergistic effect involved formation of hydroxyl radicals ( OH) and reactive chlorine species. The radical concentrations followed the order of ClO (4.8 × 10 −13 M) > OH (4.1 × 10 −13 M) > Cl (3.0 × 10 −15 M). The dominant radical was OH (>80% contribution), followed by ClO (less than18% contribution), which had relatively lower reactivity with ATZ. The synergism was pH dependent, with OH largely suppressed by 98% when the pH was acidic or basic rather than neutral, resulting in a decrease in ATZ degradation. The transformation products detected indicated that ATZ degradation involved dealkylation and dechlorination–hydroxylation, and lower yields of oxidation byproducts were obtained by ammonia/chlorine synergistic oxidation process compared to direct chlorination.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zirun Chen,Shaohong Liu,Luyi Chen,Junlong Huang,Bingna Zheng,Wen Huang,Shimei Li,Yuheng Lu,Ruowen Fu
Carbon aerogels have attracted increasing research interest in a wide range of potential applications owing to their unique structural features, yet the scalable preparation of carbon aerogels configured by nanoporous carbon skeletons with high surface area and precise pore structure is a great challenge. Herein, we report a molecular-scale interface engineering concept for high-throughput and scalable production of well-defined microporous carbon aerogels (MPCAs) based on simple and fast polycondensation (<8 s) of dialdehyde with silsesquioxane. Benefiting from the unique organic/inorganic hybrid molecule structure, the silsesquioxane favours the formation of molecular-scale silica templates with uniform carbon source/template interface. The resulting MPCAs exhibit 3D interconnected macroporous framework combined with well-defined micropore skeleton and large surface area. These intriguing features render MPCAs superb pore accessibility and utilization, and thus they demonstrate great promise as adsorbent materials for rapid removal (<10 s) of organic micropollutants with high uptake, and as electrocatalyst supports for incorporation of metal-nitrogen-carbon species with excellent activities.
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Nano Research
·
2021
·Vol. 14
·期 11
·4188-4196
·
IF 8.897
Guo Sheng-Qi,Zhang Haijun,Hu Zhenzhong,Zhen Mengmeng,Yang Bo,Shen Boxiong,Dong Fan
Semiconductor combination is one of the most common strategies to obtain high-efficiency photocatalysts; however, the effect mechanism of composition ratio on micro-structure and photocatalytic activity is remaining unclear. In this study, a case of g-C 3 N 4 quantum dots@SnS 2 (CNQD n @SnS 2 ) heterojunction with different ratio of CNQD is used to uncover the origin of optimum and excess composition for photocatalysts. Research on the functional mechanism of the optimum composition shows that 0.8 wt.% CNQD are completely attached to the non-(001) facets of SnS 2 , which benefits the formation of type-II heterojunction, resulting in an optimal pollutant degradation and mineralization efficiency. For the excess composition, both experiments and theoretical calculations confirm that excess CNQD (the part exceeding of 0.8 wt.%) located on the (001) facet of SnS 2 , leading to the type-I band alignment of this heterojunction, which severely restricts the separation of photo-induced charge carriers, and thus reduces their lifetime. This work makes the functional mechanism of composition ratio on micro-structure and photocatalytic activity clearer. Related research results provide a new insight into semiconductor combination study and take an important step toward the rational design of highly active photocatalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Rui Zhou,Haoran Song,Daoyuan Zu,Shiting Pan,Yuwei Wang,Fangxian Wang,Zhuo Li,Yongming Shen,Changping Li
The self-floating Ti 3 C 2 MXene-coated polyurethane sponge (MXene@PU module) was prepared via the simple coating operation for thermal activation of peroxydisulfate (PDS) and production of clean water. Coating MXene on the surface of PU significantly improved the degradation of model pollutant carbamazepine (CBZ) compared with PU alone under simulated solar radiation. Because of the excellent photothermal conversion performance of Ti 3 C 2 MXene and the unique double-deck structure of MXene@PU module, the interfacial temperature of MXene@PU module reached about 140 °C, far higher than that of PU (about 82 °C). Radical identification experiments demonstrated that both hydroxyl radical and sulfate radical contributed to the degradation of organic pollutant. Addition of Cl − , HPO 4 2− , HCO 3 − and natural organic matter in solution generated inhibitory effect on CBZ degradation. The prepared MXene@PU module exhibited excellent stability after long-time experiment. Importantly, the interfacial evaporation process produced abundant recycled water and no pollutant was detected in recycled water. This study provides a feasible way to utilize the renewable solar energy for removal of organic pollutants and production of clean water.
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CHEMICAL PHYSICS
·
2021
·
IF 2.348
Wenna Hu,Fan Wu,Wei Liu
In this paper, nitrobenzene was found to be efficiently degraded by the as-prepared Z-scheme Bi 2 O 3 /Bi 2 WO 6 photocatalyst under visible light . The Bi 2 WO 6 and the composites were fabricated individually by solid phase synthesis and water-assisted grinding method. The crystal structure, morphologies, interface, optical property and Brunauer-Emmett-Teller (BET) surface area of samples were examined by different characterization techniques. The tests on photodegradation of nitrobenzene stated clearly the as-prepared composite exhibited evidently enhanced photocatalytic performace compared with uniphase material. Additionally, the optimal Bi 2 O 3 content in the coupled photocatalysts was 2%. The supreme rate constant of nitrobenzene degradation was almost 3.1 and 2.7 times that of single Bi 2 O 3 and Bi 2 WO 6 , respectively. The obviously increased photocatalytic performance of the composite was due to the highly effective separation of photoexcited electron-hole pairs over the Z-scheme structure formed between Bi 2 O 3 and Bi 2 WO 6 . The investigation provides great potential applications in treatment of the toxic and refractory wastewater.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Binbin Feng,Qionghao Xu,Xiaoxue Wu,Chunlin Ye,Yanghe Fu,De-Li Chen,Fumin Zhang,Weidong Zhu
Owing to the competitive hydrogenation of reducible functionalized groups and the complexity of the reaction mechanism, the selective catalytic hydrogenation of nitroarene compounds to value-added amine products is challenging. Herein, we designed and prepared a series of highly efficient iron-based nanocomposites (Fe/Fe 3 C@NC–T) via direct pyrolysis of the presynthesized NH 2 –MIL–101(Fe) octahedrons under nitrogen atmosphere, wherein tiny metallic Fe/Fe 3 C nanoparticles (NPs) were homogeneously inlaid in the N-doped porous carbon matrix. Among the various derived catalysts, Fe/Fe 3 C@NC–750 exhibited the best performance, with good tolerance to several different functional groups for the catalytic transfer hydrogenation of nitroarenes to anilines using N 2 H 4 ·H 2 O as the reductant under mild conditions. This performance was also superior to those of commercial catalysts (Fe, Fe 2 O 3 , and Fe 3 C) and Fe/Fe 3 C@C–750 without N doping. The synergistic catalysis between the Fe-based NP and N dopant mainly contributed to the excellent catalytic performance of Fe/Fe 3 C@NC–750. Moreover, the mechanism study revealed that both the direct route and the condensation route were involved in this catalytic reaction system.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zexu Chi,Jingyun Zhao,Yi Zhang,Han Yu,Hongbing Yu
Morphology and facet engineering have been proved efficient strategies to prepare high-performance photoelectrochemical (PEC) materials. WO 3 /BiVO 4 heterojunction photoanodes with different morphologies were prepared by simply controlling the amount of electrodeposited charge. The coral-like WO 3 /BiVO 4 photoanode with the orientation growth of {110} and {011} active facets of BiVO 4 exhibited the optimal PEC performance due to significantly enhanced separation and transfer of photogenerated charge carriers, while the exposure of {−121} facets showed negative effects. 4.71 mA·cm −2 and 2.9 mA·cm −2 of photocurrent densities were obtained for sulfite and water oxidation , respectively, superior to most reported results. Subsequently, a photoelectrochemical-chlorine (PEC-Cl) system was constructed for antibiotic wastewater detoxification with hydrogen recovery. The analysis results indicated that the system can quickly and effectively remove sulfamethoxazole and reduce its toxicity concurrent with high hydrogen yield. The reactive chlorine species (RCS), especially Cl 2 · − and ClO·, dominated the sulfamethoxazole removal. Possible degradation pathways of sulfamethoxazole were also elucidated.
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