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JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY · 2019 ·Vol. 19 ·期 7 ·3879-3886 · IF 1.093

Preparation of a Pt/Active Carbon Fiber Catalyst and Its Application in the Synthesis of p-Chloroaniline with Catalytic Hydrogenation

Liu Baoliang,Yang Bing,Sun Meiyu,Qian Xiangli,Zhang Qikun

In this study, a Pt loaded active carbon fiber (Pt/ACF) catalyst was prepared by immobilizing Pt nanoparticles on ACF. The catalyst accelerated hydrogenation of p-chloronitrobenzene (p-CNB) to p-chloroaniline (p-CA) at lower temperature and atmospheric pressure, resulting in approximately 100% yield and selectivity. Several factors that affect p-CA yield were investigated. The nitro reduction rate reached 100% under the optimal reaction conditions, indicating excellent selectivity of the prepared catalyst. This process will overcome the environmental pollution problems associated with the traditional process, and is a green synthetic process.

研究领域: 化学工程 · 环境科学
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APPLIED SURFACE SCIENCE · 2017 · IF 3.387

Indium doped BiOI nanosheets: Preparation, characterization and photocatalytic degradation activity

Haibo Li,Zujin Yang,Jingnan Zhang,Yongchao Huang,Hongbing Ji,Yexiang Tong

Semiconductor photocatalysis is a promising method to remove the harmful compounds into harmless molecules. Herein, In-doped BiOI (In-BiOI) photocatalysts with highly exposed dominant {001} facets were synthesized through a facile hydrothermal method. The XRD, SEM and TEM determinations revealed the high crystallinity structure of the samples, and the XPS results confirmed the doping of In. The In-BiOI nanosheets exhibited a higher activity in the photodegradation of p -chloroaniline (PCA) than that of pristine BiOI, among which the In-2 BiOI sample (feed mole ratio of In:Bi   =   2%) possessed the best performance. Doping with In didn’t alter the structure, morphology, specific surface area or light absorption capacity of BiOI, but significantly improved its charge separation efficiency and transport capability, which were verified by the results of the lower PL emission, larger photocurrent intensity and smaller arc radius of EIS plots. More importantly, the mechanism of photocatalytic degradation is studied systematically, revealing that O 2− and h + were the major reactive species during the photodegradation process. Finally, the possible role of In-doping in enhancing the photocatalytic performance of BiOI is proposed.

CAS / MDL: 98-79-3
研究领域: 材料科学 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2018 · IF 3.927

Removal of p-chloroaniline from polluted waters using a cathodic electrochemical ceramic membrane reactor

Junjian Zheng,Shaoping Xu,Zhichao Wu,Zhiwei Wang

Degradation of p -chloroaniline (PCA) was investigated using an electrochemical reactor with Ti/SnO 2 -Sb anode and cathodic electrochemical porous ceramic microfiltration (MF) membrane under galvanostatic control. Results showed that electrochemical degradation of PCA followed pseudo-first-order kinetics. At applied current 0.8 A and membrane flux 80 L m −2  h −1 , complete degradation of PCA (initial concentration of 0.6 mM) was achieved after 90-min electrolysis following adding 0.2 mM Fe 2+ at pH 3, with 75.1% of mineralization ratio and 46.7% of total nitrogen abatement. The production of OH via either anodic water oxidation or homogeneous and surface Fenton reaction was responsible for PCA degradation. The degradation pathways of PCA involving protonation, OH oxidation, and cathodic reduction were proposed by quantifying generated organic byproducts and inorganic nitrogen ions. Compared to cross-by operation, the cross-through operated EF system exhibited an enhanced oxidation power, leading to more efficient destruction of PCA and its toxic intermediate byproducts and improving electrical energy efficiency. This was ascribed to the increased ROS production and better contact of the contaminants with ROS present in the vicinity of membrane (cathode) surface induced by the enhanced mass transfer under membrane filtration. These results highlight the potential of the cross-through operated EF system to be used for the treatment of PCA-contaminated water and wastewater.

研究领域: 环境科学 · 化学工程
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Compound specific isotope analysis to characterize degradation mechanisms of p-chloroaniline by persulfate at ambient temperature

Ning Min,Jun Yao,Meseret Amde,Cengceng Tang,Langping Wu,Hans Hermann Richnow,Yafei Chen,Yongqiang Cui,Hao Li

Compound-specific isotope analysis (CSIA) is a useful technique that has received an increasing attention for studying the degradation mechanisms of organic contaminants based on stable isotope fractionation concepts. This study reports the degradation mechanisms of p -chloroaniline (PCA) at different pH values (3, 5, 7 and 9) induced by persulfate (PS) based on 13 C isotope fractionation during its preferential oxidation with SO 4 − and OH. The results showed that the degradation of PCA followed first-order kinetics (rate constants, 0.026, 0.0362, 0.0754 and 0.0497 h −1 at pH = 3, 5, 7 and 9, respectively), with the fastest degradation under neutral conditions (pH 7). The degradation rate was found to be higher under alkaline conditions (pH 9) compared to acidic conditions (pH 3 and 5). A normal carbon isotope fractionation of PAC was observed under neutral and alkaline conditions (eg., ε C  = −0.8‰ ±0.10 at pH 7 and ε C  = −1.0‰ ±0.17 at pH 9). However, a reverse carbon isotope effect at pH 3 (ε C  = 0.6‰ ±0.07) and pH 5 (ε C  = 1.1‰ ±0.06) was observed, respectively. Based on the identified transformation products and the insights revealed by CSIA, the degradation pathways were proposed. The current findings are crucial in understanding the PCA degradation mechanisms with SO 4 − and OH in aqueous systems.

研究领域: 环境科学 · 化学
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JOURNAL OF CATALYSIS · 2022 · IF 8.047

NiOx-promoted Cu-based catalysts supported on AlSBA-15 for chemoselective hydrogenation of nitroarenes

Xiuli Li,Yuan Tan,Zongyang Liu,Juan Su,Yan Xiao,Botao Qiao,Yunjie Ding

Chemoselective hydrogenation of aromatic nitro compounds to the corresponding anilines is an environmentally benign technology for the production of key intermediates in manufacturing of pharmaceuticals, agrochemicals, dyes and fine chemicals. Non-noble metal Cu-based catalysts have been reported as a low-cost alternative but suffer from poor activity. Herein, by fabricating nickel oxide promoted Cu catalysts, a promoted activity was obtained in supported Cu-Ni bimetal catalyst system. Characterizations such as H 2 -TPR and XPS indicate a strong interaction between Cu and Ni, which contributes to its high activity and selectivity in hydrogenation of p -chloronitrobenzene ( p -CNB) to p -chloroaniline ( p -CAN). Control experiments suggest that either monometallic copper or pure nickel oxide is less active for the reaction but the interaction of NiO x with Cu generates much more active species, resulting in significantly improved catalytic reactivity and selectivity. The activity was found to be highly dependent on the contents of Cu 0 & Cu + in Cu-Ni bimetal catalyst, as the specific reaction rates for hydrogenation of p -CNB grew linearly with the increment of Cu 0 & Cu + loadings. Kinetic studies and in-situ DRIFTS of p -CNB imply the 10Cu-5Ni/AlSBA-R catalyst possesses good capacity for the activation of hydrogen and nitro group, leading to high p -CNB conversion and p -CAN production. The present work provides a good example for understanding the interaction between Cu and nickel oxides, and helps to develop highly efficient non-noble metal catalysts for selective hydrogenation of aromatic nitro compounds to corresponding anilines.

研究领域: 催化化学 · 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2018 · IF 6.735

Activation of persulfate with metal–organic framework-derived nitrogen-doped porous Co@C nanoboxes for highly efficient p-Chloroaniline removal

Ying Liu,Xiaoyan Chen,Yulin Yang,Yong Feng,Deli Wu,Shun Mao

Cobalt-based nanostructures have shown a great potential for radical production by activating persulfate (PS). Here, we report a facile strategy to synthesize nitrogen-doped porous Co@C nanoboxes (Co@NC) by pyrolysis of zeolitic imidazolate frameworks (ZIF-67), followed by partially etching away the metallic cobalt. With a nitrogen-enriched hollow porous carbon nanobox and embedded Co nanoparticles, the Co@NC shows high efficiency in PS activation for p-Chloroaniline (PCA) removal. The degradation study shows that a complete removal of high concentration PCA is done within two minutes, which is superior to most of the reported PCA removals with PS-based advanced oxidation processes (AOPs). More importantly, the Co@NC exhibits high catalytic activities in a wide range of pH from 5 to 9. The Co@NC also shows very limited Co 2+ release with a dissolution proportion of 0.28%, much lower than previously reported Co-based catalysts, and remains high efficiency after five successive reaction cycles. A heterogeneous activation mechanism though surface reaction is proposed, in which PCA firstly absorbs on the carbon nanobox surface, then being oxidized by generated radicals and non-radical species. The unique structure and outstanding performance of Co@NC catalysts present new insights in catalyst design for PS-based advanced oxidation for organic pollutants removal in waste water.

研究领域: 环境科学 · 材料科学 · 化学工程
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