Molecular Catalysis
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2024
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IF 3.9
Yalan Liu,Zhihao Zhong,Xinxin Yu,jiageng Xiong,Shantang Liu
The degradation of Chlorinated volatile organic compounds (CVOCs) by catalytic oxidation forms toxic products, and catalysts may be poisoned by chlorine at low temperatures. To address this, a Cu-assisted strategy is proposed for enhancing the catalytic degradation of chlorobenzene (CB) over cobalt oxide nanosheets. The Cu-doped Co 3 O 4 catalysts exhibited lower T 90 values (temperatures with 90 % conversion) and improved stability compared to the unmodified catalyst. These results were attributed to strong metal-metal interactions between Cu species and cobalt oxide nanosheets, which showed a high specific surface area, reduced binding energy of lattice oxygen, higher surface oxygen concentration, and more surface Co 3+ species. These properties promoted low-temperature catalytic activity. In addition, the disappearance of Cu 2+ satellite peak after the catalyst is used, indicating that the Cu 2+ also contributes to the catalytic activity. Furthermore, the in situ FTIR spectra provided details about the reaction mechanism of CB degradation over Cu-doped cobalt oxide nanosheets. The oxygen vacancy generation and the surface absorption of chlorine-containing intermediates were calculated using density functional theory calculations. This study provides new insight into novel pathways for catalyst design aimed at CB degradation.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Yaping Zhang,Guobo Li,Peng Wu,Hongqiang Yang,Sheng Wang,Kai Shen,Ling Wang
TiO 2 -Vo support with abundant oxygen vacancy was prepared by hydrothermal method, purchased TiO 2 -P for comparison, and Pd 0.12 V 4 /TiO 2 catalysts with different TiO 2 structures were prepared to investigate catalytic oxidation for dichloromethane (DCM). Pd 0.12 V 4 /TiO 2 -Vo catalyst showed excellent low temperature DCM removal efficiency, T 90 of which reduced to 290 ℃, and Cl resistance was maintained in 40 h. Abundant oxygen vacancy of TiO 2 -Vo was formed in transformation process of part anatase TiO 2 to rutile phase. The obtained Pd 0.12 V 4 /TiO 2 -Vo catalyst possessed rich acid sites, higher adsorbed oxygen (O ads ) ratio and better oxygen mobility, which inhibited loss of active components and improved DCM removal efficiency. DCM removal efficiency of Pd 0.12 V 4 /TiO 2 catalyst was reduced by HCl, while negative effect in the way of weakening competitive adsorption between HCl and DCM, that would be reduced by TiO 2 supports modification. The present work is favorable for further DCM removal catalyst anti-Cl poisoning modification and application in manufacture industry.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2024
·
IF 5.2
Jinchen Ma,Yingjie Mi,Fan Wang,Chaohe Zheng,Haodong Huang,Haibo Zhao
In the chemical looping combustion of chlorine-rich biomass or coal, a trace element, chlorine, will cause serious corrosion of oxygen carriers and heat exchange equipment in boilers. To address this issue, we design Ca- and Ba-decorated oxygen carriers to achieve two goals: on one hand, reducing the concentration of chlorine-containing gases by in situ dechlorination; on the other hand, employing protective materials to preferentially bind with gaseous chlorine to safeguard the active components of the oxygen carriers. Carefully designed experiments are conducted under simplified experimental conditions using 50 ppmv HCl-containing CH4 to evaluate the intrinsic characteristics of oxygen carriers in terms of dechlorination efficiency and reactivity. The results demonstrate that both the reaction performance and the chlorine-resistance performance of Ca–Cu and Ba–Cu composite oxygen carriers are significantly improved. This is because (a) Ca and Ba preferentially form chlorides with HCl, effectively shielding the active Cu component of the oxygen carrier from chlorine poisoning and (b) the specific surface area and pores of Ca/Ba-decorated oxygen carriers are increased, which not only strengthens the heterogeneous reaction between oxygen carrier and combustible gas but also improves the chemical looping combustion performance. The Cl-resistant oxygen carriers, Ca–Cu and Ba–Cu, emerge as promising candidates for the chemical looping combustion of fuels with high chlorine content.
研究领域:
能源化学
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材料科学
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环境工程
✓ 已验证
DOI
高影响因子
ACS Catalysis
·
2023
·
IF 12.9
Yi Liu,Fanyu Wang,Fei Xie,Jiamin Zheng,Jintong Lan,Furong Guo,Yifei Sun,Lizhi Zhang,Xiao Liu
The degradation of chlorine-containing volatile organic compounds (Cl–VOCs) utilizing catalytic combustion technology is subject to the paradox of toxic byproduct formation and catalyst chlorine poisoning. Herein, a CaO-assisted strategy is proposed to resolve the awkward stuff for improving the catalytic combustion performance of chlorobenzene on SmMn2O5. The CaO-collaborated SmMn2O5 exhibits a significant decrease in T90 by 142 and 125 °C compared with unmodified and inert SiO2-composited SmMn2O5, respectively. The integrated characterization results confirm that CaO collaboration causes electron transfer from CaO to SmMn2O5, resulting in a reduction of the orbital overlap between Mn and O atoms to activate lattice oxygen (Olatt). The activated Olatt enables chlorobenzene to combust completely at a lower temperature of 275 °C at which toxic byproducts are not generated. Furthermore, the switching of the dechlorination site from SmMn2O5 to CaO avoids chlorine poisoning of active sites on SmMn2O5 and thus endows CaO-collaborated SmMn2O5 with prominent stability.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
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2018
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IF 4.217
Shuai-wei Liu,Rui-tang Guo,Xiao Sun,Jian Liu,Wei-guo Pan,Zhi-ling Xin,Xu Shi,Zhong-yi Wang,Xing-yu Liu,Hao Qin
In present study, the poisoning mechanism of Cl on V/TiO 2 catalyst for SCR removal of NOx using NH 3 as the reductant was explored by in situ DRIFT technique. The experimental results revealed that the existence of Cl did not change the SCR reaction mechanism over V/TiO 2 catalyst, which was mainly under the control of both E-R and L-H mechanisms. The deactivation of V/TiO 2 catalyst by Cl was mainly resulted from the inhibited adsorption of NH 3 and NOx species, accompanied by the decrease of the reactivity of adsorbed NH 3 species.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Surfaces and Interfaces
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2022
·
IF 6.137
Weiquan Li,Die Hu,Ke Yin,Chenglong Yu,Bichun Huang
A series of hierarchical Ru-Ce/H-ZSM-5 were designed and synthesized using the sol-gel method, and they were applied as catalysts for the catalytic combustion of chlorobenzene. The pore diameter of the catalyst was adjusted using an amount of sodium alginate (SA). Among all of the catalysts synthesized, the 0.8 wt.%Ru-10 wt.%Ce/H-ZSM-5 catalyst with a crystallization recipe of 1SiO 2 : 0.02Al 2 O 3 : 0.15TPAOH: 0.04SA: 40H 2 O (named RCZA-0.04) exhibited the optimal catalytic activity, with the 90% conversion of chlorobenzene at 247 °C. In addition, the RCZA-0.04 catalyst maintained superb stability during a long-term reaction at 325 °C. The results of characterizations demonstrated that RCZA-0.04 possessed the largest mesoporous volume, which reduced the diffusion resistance of chlorobenzene and increased the dispersion of the active components, thereby enhancing the catalytic activities. Moreover, the RCZA-0.04 catalyst possessed a low Brønsted/Lewis ratio, which was conducive to the adsorption of chlorobenzene and the cleavage of the C Cl bond.
研究领域:
环境科学
·
催化化学
✓ 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
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化学工程
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水处理
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催化
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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）