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CHEMICAL ENGINEERING JOURNAL · 2013 · IF 3.473

Selective hydrogenation of o-chloronitrobenzene over tin dioxide supported platinum–ruthenium bimetallic nanocatalysts without solvent

Manhong Liu,Qiang Bai,Hailian Xiao,Yanyan Liu,Jun Zhao,William W. Yu

Colloidal platinum–ruthenium bimetallic nanoparticles with 2.3   nm were synthesized in solution and then immobilized on tin dioxide powder to make a supported nanocatalyst (Pt–Ru/SnO 2 ). The immobilized bimetallic nanoparticles had the same size and size distribution as the solution dispersed ones. Selective hydrogenation of o -chloronitrobenzene to o -chloroaniline was performed over the as-prepared Pt–Ru/SnO 2 nanocatalyst without using any solvent; 99.5% selectivity to o -chloroaniline at ∼100% conversion was achieved.

研究领域: 催化化学 · 纳米材料 · 有机合成 · 绿色化学 · 应用化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL · 2015 · IF 3.615

Catalytic oxidation of cyclohexane to KA oil by zinc oxide supported manganese 5,10,15,20-tetrakis(4-nitrophenyl)porphyrin

Ze Feng,Yujia Xie,Fang Hao,Pingle Liu,He'an Luo

A series of manganese metalloporphyrins were prepared and tested in cyclohexane oxidation. It has been found that the manganese 5,10,15,20-tetrakis(4-nitrophonyl) porphyrin (Mn-TNPP) presents better catalytic performance. The Mn-TNPP was then immobilized on different supports, and characterized by UV–vis, FT-IR, XRD, TG/DTG and ICP. Among these supported Mn-TNPP catalysts, Mn-TNPP/ZnO exhibits the best selectivity to KA oil and higher turnover number in cyclohexane oxidation. The influence of the reaction conditions and the recycle of the catalysts are discussed. Mn-TNPP/ZnO catalyst presents the average cyclohexane conversion of 7.17%, KA oil selectivity of 91.18%, and the average catalytic turnover number of 6.53   ×   10 4 after six times of recycle under 150   °C and 1.0   MPa.

研究领域: 催化化学 · 有机合成 · 工业化学 · 材料化学 · 绿色化学
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RSC Advances · 2016 ·Vol. 6 ·期 92 ·89821-89826 · IF 3.289

p-Nitrophenol degradation and microbial community structure in a biocathode bioelectrochemical system

Xinyu Wang,Defeng Xing,Nanqi Ren

The biocathode bioelectrochemical system (bioc-BES) was used for p-nitrophenol (PNP) degradation with sodium bicarbonate as the carbon source. The PNP degradation efficiency in bioc-BES with applied voltage of 0.5 V reached 96.1% ± 0.5% within 72 h, which was much higher than that obtained in the biocathode BES without applied voltage (bioc-BES-NAP), open circuit biocathode BES (OC-bioc-BES) or abiotic cathode BES (abioc-BES). With the increase in the PNP concentration from 20 mg L−1 to 60 mg L−1, the PNP concentration of the effluent decreased from 21.66 ± 2.94 mg L−1 to 0.38 ± 0.1 mg L−1 in 48 h. The final reductive product of PNP was p-aminophenol (PAP) in the biocathode chamber. High-throughput 454 pyrosequencing showed that predominant populations in the biocathode biofilm of bioc-BES were affiliated with electrochemically active Delftia and Diaphorobacter, while Aminobacter was the predominant population in the biocathode biofilm of the bioc-BES-NAP and OC-bioc-BES. These results suggested that microbial electrocatalysis and electrochemically active bacteria on the cathodic electrode accelerated PNP degradation in the biocathode BES (bioc-BES). The biocathode BES will be a promising treatment technology for PNP-containing wastewater.

研究领域: 环境微生物学 · 环境工程 · 生物电化学 · 污染物降解 · 废水处理 · 微生物生态学
✓ 已验证 DOI 高影响因子
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MATERIALS RESEARCH BULLETIN · 2022 · IF 5.6

Temperature-dependent Cs4PbBr6/CsPbBr3 perovskite composite for sensing 2,4-dinitriphenylhydrazine

Min Yang,Yujia Yan,Enzhou Liu,Qian Sun,Jun Fan

In recent years, all-inorganic perovskite has been extensively studied due to its excellent photoelectric properties, but the application of Cs n PbBr 2+ n perovskite with excellent stability in the field of chemical sensing has yet to be developed. Herein, Cs 4 PbBr 6 /CsPbBr 3 with good stability was successfully prepared by controlling the synthesis temperature to 100 ° C. The fluorescence intensity of Cs 4 PbBr 6 /CsPbBr 3 exhibited 2,4-dinitriphenylhydrazine (DNPH) concentration-dependent characteristics and could be used for sensing DNPH based on the dynamic quenching process triggered by the collision between Cs 4 PbBr 6 /CsPbBr 3 and DNPH. A good linear model was established based on the detection signal and DNPH concentration in the range of 0.05∼30 mg/L and the detection limit was 0.033 mg/L. This method was applied to detect DNPH in soil and tap water samples with satisfactory results obtained. Therefore, this research broadens the application of Cs n PbBr 2+ n in the field of quantitative detection and is expected to be developed into a fluorescent sensor for the detection of hydrazine substances.

研究领域: 分析化学 · 材料科学 · 环境监测 · 传感器技术 · 光电子学
✓ 已验证 DOI 高影响因子
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Journal of CO2 Utilization · 2017 · IF 4.292

A green process for production of p-aminophenol from nitrobenzene hydrogenation in CO2/H2O: The promoting effects of CO2 and H2O

Lijun Zhao,Haiyang Cheng,Tong Liu,Yan Li,Zhong Ying,Wenjing Yang,Weiwei Lin,Xiangchun Meng,Chengxue Wang,Fengyu Zhao

An efficient green process was developed for production of p -aminophenol (PAP) from hydrogenation of nitrobenzene (NB) over a traditional Pt/Al 2 O 3 catalyst in a reaction medium of supercritical CO 2 (scCO 2 ) and H 2 O without any additional acid catalyst involved. The combination of scCO 2 and H 2 O was confirmed to be effective for the production of PAP. The acidity, aroused by the in situ formed carbonic acid, increased with CO 2 pressure, which acted as acid catalysis during the reaction, and it can easily self-neutralize by depressurization of CO 2 , resulting in a green and a intensive process for it removed the final neutralization and salts disposal of the traditional liquid acids. Under the optimal reaction conditions, a high yield to PAP (68.9%) was achieved at the high conversion of NB (98.5%). Moreover, the results of in situ diffuse reflectance FTIR spectra revealed that CO was generated by the reverse water-gas shift reaction (CO 2   +   H 2   →   CO   +   H 2 O), it can adsorbed on the surface of Pt/Al 2 O 3 to suppress the undesired deep hydrogenation of N -phenylhydroxylamine (PHA) to aniline (AN), which also contributed to the obtained high selectivity of PAP. Therefore, the present green and efficient catalysis process will arouse the interest of researchers in the fields of the green and sustainable organic synthesis.

研究领域: 绿色化学 · 有机合成 · 催化化学 · 环境友好工艺 · 工业化学
✓ 已验证 DOI 高影响因子
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Fe confined in Prophyrin-based porous organic polymer as an efficient periodate activator for nonradical pathway removal of contaminants

Zhenyu Shi,Wei Zhang,Chao Qin,Yan Yan,Zhanqi Gao,Liang Zhu,Chunmei Tang,Can Jin,Shaogui Yang

Developing efficient and stable catalysts for periodate (PI) activation is important for the abatement of emerging contaminants. Herein, Fe doped into polyprophyrin-based porous organic polymer (Fe@PrPOP) was prepared via a facile one-step reaction, and its catalytic capacity and reaction mechanism for PI activation were systematically investigated. Complete removal of bisphenol A (BPA) was achieved within 12 min under the Fe@PrPOP/PI system within a wide pH range (3–8), as well as no leaching of Fe was observed throughout the reaction. Nonradical pathways, including 1 O 2 and electron transfer, were identified for the BPA removal. According to substantial characterizations and density functional theory calculations, we concluded that the scattered Fe species on the surface of Fe@PrPOP were the main active sites, which was conducive to the adsorption and activation of PI. In addition, the Fe@PrPOP/PI system exhibited selective oxidation toward various organic pollutants with electron-rich moieties. Overall, this study provides a promising alternative in activating PI for the removal of organic compounds in water.

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NEW JOURNAL OF CHEMISTRY · 2023 ·Vol. 47 ·期 11 ·5420-5430 · IF 3.3

Catalytic activation of peroxymonosulfate by Mn/N co-doped porous carbon for effective phenol degradation: crucial role of non-radical pathways

Qi Guo,Jihong Xu,Rui Tang,Yulin Min,Zhenhu Hu,Penghui Shi

In the degradation process of organic pollutants, compared with the free radical pathway, the non-radical pathway shows the advantages of mild oxidation ability, strong anti-interference, and adaptation to different pH values. In this study, a manganese–nitrogen co-doped porous carbon (Mn–N@C-1) with high nitrogen content was prepared to improve the contribution rate of non-radical pathways to the degradation process of organic pollutants. The high performance of Mn–N@C-1 is attributed to the formation of Mn–Nx sites between Pyridine N and Mn, which can effectively oxidize organic pollutants in water (phenol, bisphenol A, 2,4-dichlorophenol). In addition, the catalyst exhibits high catalytic activity over a wide pH range (pH = 3–9) and has good immunity to inorganic anions. Moreover, the Mn–Nx site and graphitic-N are considered to be the generation sites of singlet oxygen, and the role of metastable Mn–N@C-1/PMS* complexes in the electron transfer process is explored. Overall, this study explores the crucial role of non-radical pathways in the degradation of organic pollutants by carbon-based materials.

✓ 已验证 产品关联 DOI 高影响因子
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CARBOHYDRATE POLYMERS · 2023 · IF 11.2

Synthesis of porous dimethoxypillar[5]arene knitted β-cyclodextrin copolymers for efficient adsorption of organic micropollutants

Hengye Li,Xingwei Han,Wenjie Yu,Lin Zhang,Wenwen Bie,Meijie Wei,Zhongxia Wang,Fenying Kong,Wei Wang

Herein, through knitting benzylated β-cyclodextrin (BnCD) by dimethoxypillar[5]arene (P[5]), porous copolymers (P[5]-BnCDs) containing two kinds of macrocycles were synthesized with yields not <97 %. The molar ratio of P[5]/BnCD greatly influenced the P[5]-BnCDs' porosity and adsorption performance. When the molar ratio of P[5]/BnCD was 4/1, the P[5]-BnCD (4-1), demonstrated a surface area up to 515.95 m 2 /g and showed fast adsorption kinetic , high adsorption capacity and good reusability towards the model organic micropollutants (OMPs). The adsorption fitted well with the pseudo-second-order and the Langmuir models, while the thermodynamic studies revealed spontaneous physisorption process. The adsorption mechanism was dominant by host-guest and hydrophobic interactions and the adsorption at environmentally relevant concentrations experiments showed the practicality and superiority in extraction of the OMPs at μg/L level. This study paves a way for the development of versatile porous organic polymers with multiple macrocycles for efficient removal of OMPs from water.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Journal of Environmental Chemical Engineering · 2023 · IF 7.7

UV-induced degradation of contaminants of emerging concern in the presence of monobromoamine: Role of N-Br bond and degradation mechanisms

Jingxuan Yang,Dongxu Qu,Jue Wang,Yangtao Wu,Lingjun Bu,Yuanxi Huang,Shiqing Zhou

The N-Br bond in monobromoamine (NH 2 Br) can be cleaved by UV irradiation to generate Br • and subsequently HO • , resulting in an advanced oxidation condition (i.e., UV/NH 2 Br). This study investigated the degradation of six contaminants of emerging concern (CECs) in the UV/NH 2 Br process, including the phenolic hydrocarbons phenol and bisphenol A (BPA), the amines aniline and sulfadiazine (SDZ), and the persistent organic pollutants ibuprofen (IBP) and carbamazepine (CBZ). The results showed that UV/NH 2 Br process significantly improved the degradation of CECs following pseudo-first order kinetics, and the degradation of CECs was enhanced with the increase of NH 2 Br dosage. UV/NH 2 Br was more efficient in degrading CECs containing phenolic hydroxyl groups (100 %), followed by those containing amine groups (> 95 %). The degradation efficiency was influenced by the pH value and was highest at pH 7. It was found that low concentrations of Cl − (< 0.5 mM ) and HCO 3 − (< 0.5 mM) promoted the degradation of SDZ and IBP, but further increases in Cl − and HCO 3 − (0.5 ∼ 5.0 mM) resulted in inhibition. SDZ and IBP degradation was inhibited by photo absorption competition and free radical depletion in natural organic matter and actual water. Probe experiments showed that reactive bromine species (RBS), reactive nitrogen species (RNS), and hydroxyl radical (HO • ) played a dominant role in CEC degradation. During the degradation of IBP by UV/NH 2 Br, hydroxylation, bromination , and quinylation were proposed as the primary reaction mechanisms. As compared to HOCl disinfection, NH 2 Cl disinfection after the UV/NH 2 Br process produced lower concentrations of disinfection by-products (DBPs).

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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

Switching the reaction mechanisms and pollutant degradation routes through active center size-dependent Fenton-like catalysis

Xinhao Wang,Zhaokun Xiong,Hongle Shi,Zelin Wu,Bingkun Huang,Heng Zhang,Peng Zhou,Zhicheng Pan,Wen Liu,Bo Lai

Rationally regulating reaction mechanisms in Fenton-like reactions by tuning the properties of catalysts is of great significance, but still challenging. Herein, we synthesized various active center size-dependent catalysts to realize the switching of reaction mechanisms and pollutant degradation routes in peroxymonosulfate (PMS) activation systems. The results illustrated that the reaction mechanism transformed from radical oxidation (51.64%) to nonradical oxidation (89.92%) with the decrease of active center size from nanoparticle (Co NP -NC) to single atom (Co SA -NC). The evolution of reactive species switched the degradation intermediates and pathway of sulfisoxazole (SIZ). The generation of singlet oxygen ( 1 O 2 ) in Co SA -NC/PMS tends to selectively attack electron-rich site of SIZ, while reaction between radicals and SIZ prefers non-selective oxidation in Co NP -NC/PMS system. Besides, the toxicity tests indicated that the conversion from non-selective to selective oxidation resulted in lower toxicity of effluent after reaction, which can further reduce environmental risks of effluent.

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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

Cobalt–aluminum oxide clusters-embedded γ-Al2O3 nanosheets for peroxymonosulfate activation: Interfacial pH-buffering property to eliminate cobalt leaching and boost the catalytic activity

Ding Liu,Zhenkun Su,Bo Han,Kaisheng Xia,Chenggang Zhou,Qiang Gao

Cobalt–aluminum oxide clusters-embedded γ-Al 2 O 3 nanosheets (CAO@AO) were facilely fabricated and developed for peroxymonosulfate (PMS) activation. Interestingly, the Al–OH-rich amphiphilic surface of CAO@AO endowed the catalyst with unique interfacial pH-buffering property, which stabilized the reaction media at nearly neural level and thus prevented the cobalt sites from leaching. Moreover, the presence of Al–OH groups around the Co−Al oxide clusters facilitated the activation of PMS and the redox cycle of Co 2+ /Co 3+ , which resulted in a boosted catalytic activity. Consequently, the CAO@AO exhibited zero leaching of cobalt and high efficacy for PMS activation, enabling complete and ultrafast removal of metronidazole with a significantly higher turnover frequency (TOF, 1.83 min −1 ) than that of Co 3 O 4 (0.004 min −1 ). It was also demonstrated that introducing suitable foreign metal into CAO@AO could further enhance the catalytic activity (e.g., TOF of Mn(40%)-CAO@AO: 5.80 min −1 ). Furthermore, Mn(40%)-CAO@AO-decorated granular support was synthesized that dominated a continuous-flow degradation in column reaction system.

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Applied Sciences-Basel · 2023 ·Vol. 13 ·期 5 ·3182 · IF 2.7

Enhanced Heterogeneous Activation of Peroxymonosulfate by Nitrogen–Sulfur Co-Doped Mofs-Derived Carbon

Chuning Zhang,Huaqiang Chu,Qian Ma,Yanyan Chen,Jianwei Fan

It is important to further enhance the performance of green and efficient non-homogeneous catalysts for advanced oxidation process of Peroxymonosulfate (PMS-AOP) for green treatment of industrial wastewater. In this paper, nitrogen–sulfur co-doped MOFs-derived carbon material (CoSN@C) was prepared by one-pot synthesis followed by carbonization, and its morphological structure was characterized by XRD and SEM. After pyrolysis, the CoSN@C still maintained the dodecahedral morphology and structure of ZIF-67. The synergistic effects of S and N significantly elevated the activation of PMS. The results show that the CoSN@C + PMS system can effectively activate PMS to degrade Rhodamine B (RhB), with a rate constant (1.85 min−1) four times higher than that of the CoN@C + PMS system (0.44 min−1). The optimal catalytic process parameters of material dosage, PMS concentration, temperature, pH, and other parameters were also investigated for the activation of PMS to remove Rhodamine B. The cyclic experiment shows that the CoSN@C has excellent recyclability and the degradation rate of RhB still reached 88.9% after four cycles. Radical capture experiments and EPR tests showed that the CoSN@C + PMS system generated a large amount of SO4·−and ·OH radicals adsorbed on the catalyst surface and a certain amount of singlet oxygen, and the free radical pathway and non-radical pathway worked together to degrade RhB efficiently and rapidly. While non-radical pathway with singlet oxygen as main reactive oxygen species played a key role in the CoN@C + PMS system. This work provides a new idea for the rational design of non-homogeneous catalysts for PMS-AOP system.Keywords:advanced oxidation process;peroxymonosulfate (PMS);non-homogeneous catalyst;MOFs

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