SEPARATION AND PURIFICATION TECHNOLOGY
·
2015
·
IF 3.091
Jing Zhang,Yao Wu,Liping Liu,Yeqing Lan
The degradation of p -chloronitrobenzene ( p CNB) in different systems including ozone alone, ozone together with zero-valent zinc (Zn(0)) and Zn(0) bubbled with air instead of ozone was investigated. The results demonstrated that the degradation of p CNB by ozone alone was weak. However, the coexistence of Zn(0) and ozone exhibited a significantly synergistic role in p CNB degradation and approximately 98% of the initial p CNB (10 mg/L) was removed within 18 min. The degradation efficiency of p CNB was related to Zn(0) dosage and ozone flow amount, and the optimum conditions were 0.5 g/L and 4.8 mg/min, respectively. p CNB could be effectively degraded in the initial pH range of 4–10, but a higher or a lower pH was not beneficial to the removal of p CNB. Accompanying anions also affected p CNB degradation. Chloride and sulfate slightly improved p CNB degradation, whereas bicarbonate and phosphate markedly suppressed the degradation of p CNB. The reuse of Zn(0) (4 cycles) for p CNB ozonation indicated that the catalytic activity of Zn(0) maintained high and stable. The experiments of free radical scavengers ( tert -butyl alcohol and p -benzoquinone) corroborated the dominant active species responsible for p CNB degradation by a combination of ozone with Zn(0) was O 2 − rather than OH. Based on the results obtained in this study, it can be concluded that ozone activated by Zn(0) is an effective and promising approach to degrade organic contaminants.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2014
·Vol. 4
·期 23
·11788-11793
·
IF 3.708
Yanyan Fang,Hailian Xiao,Ning Sui,Manhong Liu,William W. Yu
Supported Pt nanocatalysts with controlled particle size and size distribution were prepared by immobilizing Pt colloids on different iron oxide supports (γ-Fe2O3, Fe3O4, Fe2O3) via physical adsorption. These catalysts were used to catalyze the liquid phase hydrogenation of o-chloronitrobenzene (o-CNB) to o-chloroaniline (o-CAN) under mild reaction conditions (298 K, 0.1 MPa). The Pt/γ-Fe2O3 exhibited higher catalytic selectivity and activity than other similar works (selectivity = 99.9%, activity = 0.20 molo-CNB/(molPt s)). The stability of the Pt/γ-Fe2O3 was investigated, and the result showed that higher drying temperature could increase the stability of the catalyst.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Jiutao An,Qi Wang,Xiaopu Shang,Jianli Ma,Huanzhong Bao,Dan Wu,Ying Zhang,Tiecheng Wang,Hanzhong Jia
Persulfate (PS) oxidation is a promising soil remediation technology. Information regarding pollutant degradation in soil by PS-based technique under different oxidizing atmospheres is still lacking. In this study, p -chloronitrobenzene ( p -CNB) degradation in soil in a microwave (MW) activated persulfate (MW/PS) system was evaluated under aerobic and anaerobic conditions. The experimental results demonstrated that anaerobic condition was more conducive to p -CNB degradation. Only 46% of p -CNB was degarded within 60 min treatment under aerobic conditions, but it increased to more than 80% under anaerobic conditions. The increase of PS dosage and MW temperature both promoted p -CNB degradation. SO 4 •− and •OH played important roles in p -CNB degradation under aerobic conditions, and p -CNB was mainly converted to hydroxylated byproducts including 4-nitrophenol and hydroquinone. The reductive radical S 2 O 8 •- was responsible for p -CNB degradation under anaerobic conditions, and aminated byproducts were generated. The residual toxicities of these byproducts were predicted to be decreased, compared with those of p -CNB. Furthermore, by regulating the aerobic and/or anaerobic conditions, other pollutants including pyrene and ethion were also effectively removed in the MW/PS system. Overall, this study highlighted new insights into degradation behaviors of pollutants by MW/PS treatment via aerobic and anaerobic regulation.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Huaxing Song,Geqian Fang,Zhaohua Gao,Yang Su,Xiaorui Yan,Jian Lin,Wenhua Wang,Wanzhong Ren,Haisheng Wei
Supported metal catalysts play a significant role in heterogeneous catalysis in liquid phase reaction systems, but they usually suffer from a stability problem. Encapsulation of active metal species without the compromise of catalytic performance has been considered as an effective strategy. Here, we report an ultrastable Ru-based catalyst with particle size of around 1.1 nm for selective hydrogenation reaction. The highly dispersed Ru species are covered by the in situ formed porous N–C–ZnO overlayer, which is induced through the transforming of ZIF-8 shell that derives from a ZnO substrate. The resulting Ru/ZnO@N–C–ZnO catalyst can exhibit good stability in the hydrogenation of p-chloronitrobenzene after 20 cyclic runs with 100% selectivity toward p-chloroaniline. Comparatively, the naked Ru/ZnO catalyst with larger Ru particles shows serious metal leaching issue with inferior stability and poor selectivity. It is revealed that the excellent performance of Ru/ZnO@N–C–ZnO is attributed to the porous overlayer, which strengthens the bonding of Ru nanoparticles on ZnO.
研究领域:
催化
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材料科学
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化学工程
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2014
·Vol. 5
·期 1
·405-414
·
IF 4.76
Hongmei Liu,Kai Tao,Chunrong Xiong,Shenghu Zhou
In this work, Pd–NiO@SiO2 core–shell mesoporous nanocatalysts with ~4 nm Pd–NiO heteroaggregate nanoparticle cores and ~17 nm mesoporous silica shells were successfully synthesized by a sol–gel method. The surfactant-capped PdNi alloy nanoparticles were coated with SiO2 through hydrolysis of tetraethylorthosilicate to obtain PdNi@SiO2 nanoparticles, and the mesoporous Pd–NiO@SiO2 core–shell nanocatalysts were formed after removal of surfactants by calcination at 500 °C and subsequent H2 reduction at 200 °C. The characterization results by XRD, TEM and BET revealed that Pd–NiO@SiO2 nanocatalysts were highly stable with the maintenance of intact core–shell structures under high-temperature thermal treatments. The Pd–NiO@SiO2 nanocatalysts illustrated a superior catalytic performance for p-chloronitrobenzene hydrogenation with H2 to the control Pd@SiO2 nanocatalysts. The catalytic performance enhancement of Pd–NiO@SiO2 nanocatalysts is ascribed to the strong interaction between Pd and NiO in the cores, where the interfaces may be beneficial for hydrogenation reactions.
研究领域:
材料科学
·
化学工程
·
纳米技术
·
催化
✓ 已验证
产品关联
DOI
高影响因子
WATER SCIENCE AND TECHNOLOGY
·
2019
·Vol. 80
·期 5
·902-910
·
IF 1.624
Qun W.,Jingnan Z.,Hong L.,Mengling L.,Xiaohui L.,Zhichao Y.,Tao H.,Pengyu W.
In this study, a mesoporous TiO 2 /carbon catalyst (TiO 2 /C) was prepared by a facile impregnation-carbonization approach to catalyze ozonation of p -chloronitrobenzene ( p -CNB). The catalyst was well characterized and the catalytic efficiency under various conditions was systematically evaluated. TiO 2 /C has a disordered mesostructure with a high specific surface area. 92.8% of p -CNB (2 μmol/L) can be degraded within 20 min in the TiO 2 /C/O 3 system in the presence of 1 mg/L O 3 , 100 mg/L catalyst, at pH = 5. Based on the evaluation of the effect of basic parameters, it could be deduced that the removal of p -CNB relied on the synthetic effect of catalysis by TiO 2 /C and the autocatalytic induction of p -CNB. The removal efficiency of p -CNB, the structure change and the leaching of Ti ions were also evaluated in five cycles, indicating TiO 2 /C is stable and recyclable for catalytic ozonation in water treatment.
研究领域:
环境科学
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催化化学
·
水处理技术
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材料科学
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环境工程
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纳米材料应用
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Tianhao Li,Shiwei Wang,Hongbo Yu,Luohao Yuan,Dengsong Zhang,Hongfeng Yin
Restricting reactive metal nanoclusters into a microporous zeolite matrix (metal@zeolite) can not only prevent the sintering of metal species but can also regulate their catalytic selectivities to certain products. However, there are some problems with current synthesis methods for these structures, such as low metal utilization or/and low product yield. Herein, we report a general strategy to encapsulate different noble metal nanoclusters (e.g., Pd, Pt, Rh, and Ru) into various zeolites (e.g., S-1, ZSM-5, SSZ-13, NaA, and beta). The key point of this strategy is the soft gel precursor (H2O/Si < 4) in the posthydrolysis evaporation process, which significantly improves metal utilization. Combined with the high temperature crystallization process, the space-time yield has been significantly improved, simultaneously. As a typical example, the metal utilization and space-time yield of Pd@S-1 synthesized through this method were nearly 2 and 67 times higher than those of the typical hydrothermal route, respectively. Compared with a supported Pd/SiO2 nanocatalyst, Pd@S-1 exhibited higher catalytic activity and selectivity in hydrogenation of p-chloronitrobenzene (p-CNB).
研究领域:
材料科学
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催化
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化学工程
✓ 已验证
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Wang Zhe,Wang Chunpeng,Mao Shanjun,Lu Bing,Chen Yuzhuo,Zhang Xie,Chen Zhirong,Wang Yong
Decoupling the electronic and geometric effects has been a long cherished goal for heterogeneous catalysis due to their tangled relationship. Here, a novel orthogonal decomposition method is firstly proposed to settle this issue in p -chloronitrobenzene hydrogenation reaction on size- and shape-controlled Pt nanoparticles (NPs) carried on various supports. Results suggest Fermi levels of catalysts can be modulated by supports with varied work function ( W f ). And the selectivity on Pt NPs of similar size and shape is linearly related with the W f of support. Optimized Fermi levels of the catalysts with large W f weaken the ability of Pt NPs to fill valence electrons into the antibonding orbital of C–Cl bond, finally suppressing the hydrodehalogenation side reaction. Foremost, the geometric effect is firstly spun off through orthogonal relation based on series of linear relationships over various sizes of Pt NPs reflecting the electronic effect. Moreover, separable nested double coordinate system is established to quantitatively evaluate the two effects.
研究领域:
催化
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化学工程
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY
·
2017
·Vol. 17
·期 6
·3744-3750
·
IF 1.483
Yang Guangming,Yu Hongbo,Zhang Jianfeng,Yin Hongfeng,Ma Zhen,Zhou Shenghu
AuPd nanoparticles (NPs) protected by tetradecyl trimethyl ammonium bromide (TTAB) were coated with SiO2 through hydrolysis of tetraethylorthosilicate (TEOS). The as-synthesized AuPd@SiO2 core–shell NPs were calcined in air at 500 °C to remove TTAB and
open up mesopores within the SiO2 shells. The obtained Au–PdO@m-SiO2 NPs were reduced by H2 at 300 °C to obtain AuPd@m-SiO2 NPs with AuPd NP cores (diameter: ~3 nm) and SiO2 shells (thickness: ~18 nm). Results from relevant characterization
indicated that these SiO2-protected core–shell NPs were highly stable during calcination and subsequent reduction. Au@m-SiO2, Au10Pd@m-SiO2, Au5Pd@m-SiO2, AuPd5@m-SiO2, AuPd10@m-SiO2,
and Pd@m-SiO2 NPs with similar core sizes and shell thicknesses were also synthesized. These samples were tested in the catalytic hydrogenation of p-chloronitrobenzene. The activity and selectivity were found to be tunable, depending on the composition of the bimetallic alloys.
AuPd@m-SiO2 NPs with a 1/1 molar ratio of Au/Pd showed the highest selectivity for the hydrodechlorination of p-chloronitrobenzene.
研究领域:
材料科学
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催化
·
化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2022
·Vol. 16
·期 12
·1782-1792
·
IF 4.803
Lin Yuemin,Zhang Yuanyuan,Nie Renfeng,Zhou Kai,Ma Yao,Liu Mingjie,Lu Dan,Bao Zongbi,Yang Qiwei,Yang Yiwen,Ren Qilong,Zhang Zhiguo
Ultra-dispersed Ni nanoparticles (7.5 nm) on nitrogen-doped carbon nanoneedles (Ni@NCNs) were prepared by simple pyrolysis of Ni-based metal—organic-framework for selective hydrogenation of halogenated nitrobenzenes to corresponding anilines. Two different crystallization methods (stirring and static) were compared and the optimal pyrolysis temperature was explored. Ni@NCNs were systematically characterized by wide analytical techniques. In the hydrogenation of p -chloronitrobenzene, Ni@NCNs-600 (pyrolyzed at 600 °C) exhibited extraordinarily high performance with 77.9 h −1 catalytic productivity and > 99% p -chloroaniline selectivity at full p -chloronitrobenzene conversion under mild conditions (90 °C, 1.5 MPa H 2 ), showing obvious superiority compared with reported Ni-based catalysts. Notably, the reaction smoothly proceeded at room temperature with full conversion and > 99% selectivity. Moreover, Ni@NCNs-600 afforded good tolerance to various nitroarenes substituted by sensitive groups (halogen, nitrile, keto, carboxylic, etc.), and could be easily recycled by magnetic separation and reused for 5 times without deactivation. The adsorption tests showed that the preferential adsorption of −NO 2 on the catalyst can restrain the dehalogenation of p -chloronitrobenzene, thus achieving high p -chloroaniline selectivity. While the high activity can be attributed to high Ni dispersion, special morphology, and rich pore structure of the catalyst.
研究领域:
化学工程
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催化
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材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Changjin Ou,Sujuan Yuan,Fujii Manabu,Ke Shi,Mohamed Elsamadony,Juntong Zhang,Juan Qin,Jian Shi,Zhipeng Liao
Anaerobic biotechnology for wastewaters treatment can nowadays be considered as state of the art methods. Nonetheless, this technology exhibits certain inherent limitations when employed for industrial wastewater treatment, encompassing elevated substrate consumption, diminished electron transfer efficiency, and compromised system stability. To address the above issues, increasing interest is being given to the potential of using conductive non-biological materials, e,g., iron sulfide (FeS), as a readily accessible electron donor and electron shuttle in the biological decontamination process. In this study, Mackinawite nanoparticles (FeS NPs) were studied for their ability to serve as electron donors for p -chloronitrobenzene ( p -CNB) anaerobic reduction within a coupled system. This coupled system achieved an impressive p -CNB removal efficiency of 78.3 ± 2.9% at a FeS NPs dosage of 1 mg/L, surpassing the efficiencies of 62.1 ± 1.5% of abiotic and 30.6 ± 1.6% of biotic control systems, respectively. Notably, the coupled system exhibited exclusive formation of aniline (AN), indicating the partial dechlorination of p -CNB. The improvements observed in the coupled system were attributed to the increased activity in the electron transport system (ETS), which enhanced the sludge conductivity and nitroaromatic reductases activity. The analysis of equivalent electron donors confirmed that the S 2- ions dominated the anaerobic reduction of p -CNB in the coupled system. However, the anaerobic reduction of p -CNB would be adversely inhibited when the FeS NPs dosage exceeded 5 g/L. In a continuous operation, the p -CNB concentration and HRT were optimized as 125 mg/L and 40 h, respectively, resulting in an outstanding p -CNB removal efficiency exceeding 94.0% after 160 days. During the anaerobic reduction process, as contributed by the predominant bacterium of Thiobacillus with a 6.6% relative abundance, a mass of p -chloroaniline ( p -CAN) and AN were generated. Additionally, Desulfomonile was emerged with abundances ranging from 0.3 to 0.7%, which was also beneficial for the reduction of p -CNB to AN. The long-term stable performance of the coupled system highlighted that anaerobic technology mediated by FeS NPs has a promising potential for the treatment of wastewater containing chlorinated nitroaromatic compounds, especially without the aid of organic co-substrates.
研究领域:
环境工程
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生物技术
·
废水处理
·
化学工程
·
微生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Long Chen,Li-Ting Zhou,Yang-Cheng Ding,Di Wu,Hua-Jun Feng
As an important raw material for the synthesis of chemical and pharmaceutical, hazardous carcinogen p-chloronitrobenzene ( p -CNB) has been widely found in high-salinity wastewater which need to be treated carefully. Due to the high-salinity shock on microorganisms , conventional microbial treatment technologies usually show poor effluent quality. This study initially investigated the p -CNB removal performance of microorganisms stimulated by 1.2 V low-voltage in high-salinity wastewater under facultative anaerobic conditions and further revealed the enhanced mechanisms. The results showed that the p -CNB removal kinetic parameter k p-CNB in the electrostimulating microorganism reactor (EMR) increased by 104.37 % to 155.30 % compared to the microorganism reactor (MR) as the control group under the varying salinities (0–45 g/L NaCl). The secretion of extracellular polymeric substances (EPS) in halotolerant microorganisms mainly enhanced by 1.2 V voltage stimulation ranging from 0 g/L NaCl to 30 g/L NaCl. Protein concentration ratio of EMR to MR in loosely bound EPS achieved maximum value of 1.77 at the salinity of 15 g/L NaCl, and the same ratio in tightly bound EPS also peaked at 1.39 under the salinity of 30 g/L NaCl. At the salinity of 45 g/L NaCl, 1.2 V voltage stimulation mainly enhanced salt-in strategy of halotolerant microorganisms, and the intracellular Na + and K + concentration ratio of EMR to MR reached maximum and minimum values of 0.65 and 1.92, respectively. Furthermore, the results of microbial metagenomic and metatranscriptomic analysis showed the halotolerant microorganisms Pseudomonas_A and Nitratireductor with p -CNB removal ability were enriched significantly under 1.2 V voltage stimulation. And the gene expression of p -CNB removal, salt-in strategy and betaine transporter were enhanced under voltage stimulation at varying salinities. Our investigation provided a new solution which combined with 1.2 V voltage stimulation and halotolerant microorganisms for the treatment of high-salinity wastewater.
研究领域:
环境工程
·
微生物学
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废水处理
·
生物技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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