NEW JOURNAL OF CHEMISTRY
·
2015
·Vol. 40
·期 1
·372-376
·
IF 3.086
Weidong Jiang,Zhen Xiang,Bin Xu,Xiaojing Li,Fuan Liu,Guangyin Fan
Uniformly dispersed Pd nanoparticles supported on reduced graphene oxide (RGO) have been conveniently synthesized by a facile one-pot approach through the co-reduction of sodium tetrachloropalladate(II) and graphene oxide (GO) using NaBH4 as the reducing agent. The catalytic activity of Pd/RGO was investigated for aqueous hydrodechlorination (HDC) of chlorophenols at room temperature using hydrogen balloon pressure without any additives. Results indicated that Pd/RGO exhibited an excellent activity with a reaction rate of 280.0 min−1 gpd−1 for the hydrodechlorination (HDC) of 4-CP. Furthermore, the Pd nanoparticles supported on RGO can be easily recovered and reused for four times without any obvious leaching and loss of activity.
研究领域:
化学
·
环境科学
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DOI
高影响因子
CATALYSIS LETTERS
·
2024
·Vol. 155
·期 1
·1-15
·
IF 2.3
Gao Qing,Yu Yingxue,Wang Chengyun,Xiang Rui,Lu Hao
Designing an efficient Pd-based catalyst with high atom utilization efficiency is a pressing priority, presenting a significant challenge for the practical deployment of electrocatalytic hydrodechlorination (EHDC), a promising method for degrading hazardous chlorophenols (CPs). Herein, a hybrid Pd/Co(OH) 2 /NF electrode for the dechlorination of 2,4- dichlorophenol (2,4-DCP) is fabricated by a newly developed etching-deposition approach. Physical characterizations demonstrate that ultra-fine Pd nanoparticles (1.57 ± 0.29 nm) accompany with Pd 2+ hydroxides are uniformly deposited on the surface of Co(OH) 2 nanowire arrays. EHDC tests on Pd/Co(OH) 2 /NF show an impressive catalytic performance with a 94.5% removal efficiency within 2 h, fast reaction kinetics (0.024 min − 1 ) and remarkable current efficiency (55.4%), highly competitive with literature reports. Mechanism investigations indicate that the even distribution of Pd nanoparticles and coexistence of Pd 2+ sites facilitate the production of active H * and activation of C-Cl, contributing to the improvement of activity.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
RSC Advances
·
2014
·Vol. 4
·期 48
·25440-25446
·
IF 3.708
Yanlin Ren,Guangyin Fan,Weidong Jiang,Bin Xu,Fuan Liu
Magnetic palladium/reduced graphene oxide nanocomposites (Pd/rGO-Fe3O4) were prepared by depositing Pd nanoparticles on an rGO-Fe3O4 magnetic support. The as-prepared nanocomposites were investigated as catalysts for the hydrodechlorination of 4-chlorophenol in the aqueous phase. The complete conversion of 4-chlorophenol (with a concentration as high as 2.5 g L−1) to phenol was obtained in a reaction time of 40 min at room temperature and balloon hydrogen pressure without any additives. The excellent catalytic activity of the Pd/rGO-Fe3O4 can be attributed to the small particle size of Pd, and an electron-deficient state of Pd in the catalyst as a result of the strong interaction between the active sites and the oxygen of the oxygen-containing groups on the rGO-Fe3O4 support.
研究领域:
环境科学
·
催化化学
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DOI
高影响因子
ENERGY & FUELS
·
2025
·
IF 5.3
Qingxiang Zhang,Dengqian Zhang,Zhen Wang,Zheng Liu,Yukun Xi,Wei Zhang,Chen Zhang,Yin Liu
Catalytic transfer hydrodechlorination of plastic pyrolysis oil on supported transition-metal catalysts using isopropanol as a hydrogen donor was investigated in this work. The catalysts were characterized by N2 adsorption, X-ray diffraction, hydrogen temperature-programmed desorption, and X-ray photoelectron spectroscopy, and the reaction products were identified by GC-MS. Among various Al2O3-supported transition-metal (Cu, Co, Ni) catalysts, Cu/Al2O3 exhibited the best catalytic transfer hydrodechlorination performance due to the superior activation ability of Cu/Al2O3 for isopropanol. The doping of Ni in Cu/Al2O3 significantly enhanced its catalytic activity due to the inherent excellent hydrogenation activity of Ni, good metal dispersion, and strong Ni–Cu interaction in Ni–Cu/Al2O3. GC-MS results revealed that chlorobenzene was hydrogenated to benzene and HCl, and isopropanol was dehydrogenated to form acetone, which was subsequently transformed to methyl isobutyl ketone. The reactivities of three representative organochlorine compounds followed the order of chlorobenzene > tetrachloroethane > tetrachloroethylene. Ultradeep dechlorination of real plastic pyrolysis oil was achieved by catalytic transfer hydrodechlorination over the optimal 15Ni-10Cu/Al2O3 catalyst. The chlorine content of real plastic pyrolysis oil was reduced from 61.7 to 0.5 mg/L with a chlorine removal of 99.2% after reaction for 3 h at the reaction temperature of 210 °C.
研究领域:
化学工程
·
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Shuang Wu,Zheni Wang,Lei Wan,Chenghui Luo,Shams Ali Baig,Xinhua Xu
In the present study, Pd/Ni foam electrode was prepared by improved impregnation method for electrocatalytic hydrodechlorination (ECH) of clofibric acid (CA). The effects of complexing agent addition into the impregnation solution for the formation of Ni(OH) 2 and the ECH activity of Pd/Ni foam electrode were investigated. Results revealed that the introduction of sodium acetate (the complexing agent) greatly enhanced the ECH activity as compared to common impregnation liquid. Characterizations analyses demonstrated that the addition of sodium acetate did not change the phase of the electrode’s surface, but effectively reduced the deposition of Ni(OH) 2 . The surface morphology of the electrode was changed simultaneously by the addition of sodium acetate and the interlacing structure of Ni(OH) 2 and Pd catalyst was formed. NaAc before -Pd/Ni and NaAc after -Pd/Ni foam electrodes were used to perform ECH experiments on CA, and the combined Pd/Ni foam 15 min electrode was compared with the Pd/Ni foam 6 h electrode. After 2 h of electrolysis, the NaAc after -Pd/Ni foam electrode was found to remove the CA (∼100%) in the solution, which was 1.3 times the removal rate of the Pd/Ni foam 6 h electrode to CA and exceeded the Pd/Ni foam 15 min electrode. Findings from the present study demonstrated that adding the complexing agent into the impregnation solution can improve the ECH activity of Pd/Ni foam electrode and achieve a faster and more efficient dechlorination effect of CA.
研究领域:
环境化学
·
电化学
·
催化
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
·
2021
·
IF 5.097
Tao Hu,Tingting Liu,Caiyun Xu,Mingxi Liu,Shenghu Zhou
In this study, we for the first time use ditopic bis-terpyridine-containing metallopolymers as templates to synthesize metal nanoparticle-encapsulated nanoreactors. In the presence of the surfactant cetyltrimethylammonium bromide, the ditopic bis-terpyridines coordinate Pd2+ ions to form linear metallopolymer bundles, which are further used as templates for silica deposition to give silicified Pd ion-containing tubular metallopolymers. The following calcination and subsequent reduction simultaneously result in Pd NP-encapsulated silica nanotubes (Pd-SNTs). Relative to the silica-supported Pd catalysts, the prepared Pd-SNTs demonstrate enhanced performance for hydrodechlorinations of various chlorophenols into phenolic compounds at 35 °C and atmospheric H2 pressure and present high catalytic stability during five cycles of hydrodechlorination reactions.
研究领域:
材料科学
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催化
·
纳米技术
·
环境化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yun Fan,Haijun Zhang,Meihui Ren,Yichi Zhang,Yun Li,Longxing Wang,Jiping Chen
It is of great significance to develop the low-temperature catalysts for the reduction in emission of chlorinated aromatic hydrocarbons (CAHs) from the industrial thermal processes. In this work, the bimetallic Ce-Zr/UiO-66 catalysts were synthesized by a solvothermal method to degrade CAHs. Powder X-ray diffraction, Fourier transform infrared spectra and X-ray photoelectron spectroscopy analyses showed that cerium was successfully incorporated into the lattice of Zr/UiO-66 without destroying the structure of metal–organic frameworks. The activities of Ce-Zr/UiO-66 catalysts for CAHs degradation varied with the concentration of cerium. Ce 0.2 Zr 0.8 /UiO-66 with the highest surface area (1502 m 2 g −1 ) presented the highest efficiency (>85%) for hexachlorobenzene degradation at low heating temperature (100–150 °C) with less formation of polychlorinated dibenzo- p -dioxins and dibenzofurans. Appropriate amount of water (5 wt%) and nitrogen atmosphere were beneficial to improve degradation efficiency. The degradation products proved that hydrodechlorination and oxidation of CAHs both occurred on the catalysts.
研究领域:
环境化学
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催化
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材料科学
✓ 已验证
DOI
高影响因子
Catalysts
·
2024
·Vol. 14
·期 7
·424
·
IF 3.8
Mingyue Liu,Gang Chen,Zhenjun Song,Zhicai He,Aiguo Zhong,Mei Cui
Catalytic dechlorination of organic chlorides by palladium (Pd) with HCOOH represents one of the most effective and promising techniques for environmental remediation. In this study, we adopted alkaline-modified porous natural sponge as support of a Pd nanocatalyst (Pd@M-Sponge) and HCOOH as a hydrogen source for the hydrodechlorination of florfenicol (FF),o-chlorophenol (o-CP), andp-chlorophenol (p-CP). Favorable conversion efficiency of FF,o-CP, andp-CP was achieved at 25 °C and atmospheric pressure attributed to the small diameter and high catalytic reactivity of the prepared Pd NPs, in addition to the slight internal mass transfer limitation of the prepared Pd@M-Sponge. High reaction rate constants were obtained even in the conditions of a low molar ratio of HCOOH top-CP (10:1) and a high concentration ofp-CP (500 mg/L). The prepared catalyst also demonstrated superior recyclability without any obvious decrease in catalytic reactivity in 20 successivep-CP dechlorination cycles. This work provides an ideal recyclable and cost-effective catalyst based on renewable and biocompatible natural material for the catalytic hydrodechlorination of chlorinated organic pollutants with formic acid and a new view for the exploration and designing of highly reactive and stable catalysts for hydrodechlorination.
研究领域:
环境科学
·
催化
·
纳米技术
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 18
·8785-8796
·
IF 3.3
Jiaxin Zhang,Xianlang Chen,Jinhua Yu,Zheng Fang,Lele Yan,Zijian Wang,Zhengyu Pan,Rongrong Li,Li Zhang
Catalytic hydrodechlorination (HDC) is considered as one of the most promising strategies for the treatment of chlorinated environmental pollutants. Here we proposed a strategy for rapid complete dechlorination by exploiting a B–N co-doped hierarchically porous carbon material (BNC) to immobilize Pd NPs, which makes use of not only the micro/meso porous structure to accelerate the mass transport and to provide enormous active sites, but also the synergistic effect for codoping of B–N to enhance the interaction between Pd NPs and support and thus to stabilize and disperse the small size of the Pd particle. Ascribed to these combined advantages, Pd/BNC exhibited more distinctive catalytic dehalogenation activity (k = −0.14 min−1) and better stability (about 90.0% activity retention after 5 cycles) than Pd/C (k = −0.0070 min−1). Additionally, density functional theory (DFT) calculation indicates that the incorporation of N and B atoms in the carbon skeleton will reduce the adsorption energy of Cl− and thus Pd/BNC exhibits more remarkable stability than Pd/C during long-term HDC reactions. As a result, ultrafine Pd particles and high Pd2+/(Pd2+ + Pd0) ratios were found in Pd/BNC.
研究领域:
环境科学
·
材料科学
·
催化
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
WATER RESEARCH
·
2022
·
IF 13.4
Lin Hu,Li Shi,Fei Shen,Qiuwen Tong,Xiaoshu Lv,Yiming Li,Zixun Liu,Liang Ao,Xianming Zhang,Guangming Jiang,Li'an Hou
The high salinity and coexistence of scaling ions (Ca 2+ , Mg 2+ , HCO 3 − ) in wastewater challenge the efficacy and durability of palladium (Pd)-mediated electrocatalytic hydrodechlorination (EHDC) reaction for chlorinated organic pollutant detoxification, due to the accompanying Cl − poisoning at Pd sites and scaling on electrode. In a concentrated NaCl solution (5.8 g L − 1 ) with Ca 2+ (80.0 mg L − 1 ), Mg 2+ (30.0 mg L − 1 ) and HCO 3 − (180.0 mg L − 1 ), the EHDC efficiency of Pd towards 2,4-dichlorophenol decreases significantly from 67.8% to 33.1% in 72.0 h of reaction, and the electrode is covered with layers of fluffy aragonite precipitate. Herein we demonstrate the inclusion of a commercial antiscalant 2-phosphonobutane-1,2,4-tricarboxylic acid (PBTC) can prevent both scale formation and Cl − poisoning, leading to an efficient and steady EHDC process. A mechanistic study reveals that the unique dual function of PBTC primarily originates from the bearing phosphonate and carboxyl groups. With the large affinity of these groups (especially the phosphonate group) for scaling cations and Pd, the PBTC can chelate and stabilize the scaling cations in water and replace Cl − at Pd surface. It can also release protons, and trigger the formation of more electron-deficient Pd δ+ species via PBTC-Pd binding, leading to an enhanced EHDC. This work provides effective solutions to the scaling/poisoning issues that commonly encountered in real wastewater and paves a solid road for EHDC application in pollution abatement.
研究领域:
环境工程
·
化学工程
·
水处理
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催化
·
废水管理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）