ENERGY & FUELS
·
2024
·
IF 5.2
Wenbo Jia,Yueyuan Wang,Shaohua Ling,Liren He,Binghe Chen,Songtao Liu,Chuanmin Chen,Yue Cao
Fast selective catalytic reduction (SCR) atmosphere can significantly improve the NOx removal activity of VWTi catalysts, while the catalytic performance and reaction pathway of Hg0 oxidation in a fast SCR atmosphere are still unclear. In this paper, the catalytic activity of simultaneous NOx removal and Hg0 oxidation over VWTi catalysts in a simulated fast SCR atmosphere was investigated for the first time. The results showed that VWTi catalysts possessed a wide NOx removal active temperature window and a high Hg0 oxidation activity in a fast SCR atmosphere. The X-ray photoelectron spectroscopy (XPS) and Hg temperature-programmed desorption (Hg-TPD) methods were used to investigate the Hg0 oxidation process over VWTi catalysts in a fast SCR atmosphere. Combined with the homogeneous Hg0 oxidation experiment results, two domination reaction routes of Hg0 oxidation over VWTi catalysts in a fast SCR atmosphere were proposed. One was that the adsorbed Hg0 could react with the surface active species to form HgO. The other reaction route was a gaseous homogeneous route that the gaseous Hg0 could be oxidized directly to Hg(NO3)2 by gaseous NO2. Particularly, the gaseous homogeneous Hg0 oxidation process could notably weaken the inhibition effect of NH3 on Hg0 oxidation, thus improving the Hg0 oxidation activity of VWTi catalysts in a fast SCR atmosphere.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
APPLIED ENERGY
·
2019
·
IF 8.426
Haitao Zhao,Collins I. Ezeh,Weijia Ren,Wentao Li,Cheng Heng Pang,Chenghang Zheng,Xiang Gao,Tao Wu
The detrimental impact of urban airborne Hg 0 from fossil fuel utilization has necessitated the discovery and development of Hg 0 sensing materials for effective Hg 0 detection and mitigation of the pollutant. Earlier studies have hypothetically and experimentally supported 2-dimensional transition-metal dichalcogenides (2D TMDCs), particularly MoS 2 to have excellent performance for Hg 0 removal. However, the potential of other TMDCs is yet to be investigated for Hg 0 sensor application. In this study, a total of 28 transition metals within periods 4–6 of the periodic table, excluding the lanthanides series, were examined. To ensure proper data management flow, a high-throughput data mining approach with integrated machine learning and cheminformatics simulation approaches is developed. The systemic approach integrates the Pymatgen, Factsage, Aflow and density functional theory simulation tools for accelerated discovery of suitable TMDCs from raw data via the chemical vapour reaction route. Predicted results showed that TiS 2 , NiS 2 , ZrS 2 , MoS 2 , PdS 2 and WS 2 exhibited TMDCs characteristics. Furthermore, first-principles calculation shows Hg-uptake capacity is in the order NiS 2 > PdS 2 > TiS 2 > ZrS 2 > WS 2 > MoS 2 , while Hg sensing response is in the order PdS 2 > MoS 2 > WS 2 > ZrS 2 > NiS 2 > TiS 2 . Accordingly, PdS 2 depicted to be the most suitable TMDCs for airborne Hg 0 sensor application. The proposed systemic approach is an initial platform for materials discovery using integrated machine learning approaches and is well-suited for the screening and the discovery of new materials based on component-oriented structures.
研究领域:
材料科学
·
环境科学
·
化学信息学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2018
·Vol. 25
·期 21
·20575-20590
·
IF 2.8
Lu Pei,Yue Huifang,Xing Yi,Wei Jianjun,Zeng Zheng,Li Rui,Wu Wanrong
In this study, series of Ce x Zr y Mn z O 2 /r-Al 2 O 3 catalysts were prepared by impregnation method and explored to co-purification of NO x and Hg 0 at low temperature. The physical and chemical properties of the catalysts were investigated by XRD, BET, FTIR, NH 3 -TPD, H 2 -TPR, and XPS. The experimental results showed that 10% Ce 0.2 Zr 0.3 Mn 0.5 O 2 /r-Al 2 O 3 yielded higher conversion on co-purification of NO x and Hg 0 than the other prepared catalysts at low temperature, especially at 200–300 °C. 91% and 97% convert rate of NO x and Hg 0 were obtained, respectively, when 10% Ce 0.2 Zr 0.3 Mn 0.5 O 2 /r-Al 2 O 3 catalyst was used at 250 °C. Moreover, the presence of H 2 O slightly decreased the removal of NO x and Hg 0 owing to the competitive adsorption of H 2 O and Hg 0 . When SO 2 was added, the removal of Hg 0 first increased slightly and then presented a decrease due to the generation of SO 3 and (NH 4 ) 2 SO 4 . The results of NH 3 -TPD indicated that the strong acid of 10% Ce 0.2 Zr 0.3 Mn 0.5 O 2 /r-Al 2 O 3 improved its high-temperature activity. XPS and H 2 -TPR results showed there were high-valence Mn and Ce species in 10% Ce 0.2 Zr 0.3 Mn 0.5 O 2 /r-Al 2 O 3 , which could effectively promote the removal of NO x and Hg 0 . Therefore, the mechanisms of Hg 0 and NO x removal were proposed as Hg (ad) + [O] → HgO (ad), and 2NH 3 /NH 4 + (ad) + NO 2 (ad) + NO (g) → 2 N 2 + 3H 2 O/2H + , respectively.
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研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
PubMed
高影响因子
FUEL
·
2015
·
IF 3.52
Ting Liu,Lucheng Xue,Xin Guo
A series of elemental mercury removal experiments were performed at different temperatures to explore the elemental mercury oxidation efficiency on α-Fe 2 O 3 and γ-Fe 2 O 3 in the presence of H 2 S. Our experimental results indicated that the α-Fe 2 O 3 and γ-Fe 2 O 3 similarly played important roles in removing elemental mercury. The reaction temperature around 230 °C is a critical turning point in effectively capturing elemental mercury, above which the Hg 0 removal efficiency would decrease. According to our previous researches, H 2 S will preferentially adsorb on the Fe 2 O 3 surface, forming active sulfur sites to react with Hg 0 . In this paper, we analyzed the contrastive samples before and after removing Hg 0 to further investigate the probable products by the Hg 0 re-release experiments, as well as thermogravimetry–differential scanning calorimeter (TG–DSC) and X-ray photoelectron spectroscopy (XPS) analysis. The test results of morphological characterization showed that mercury compounds and new substances generated in the Fe 2 O 3 samples after adsorbing Hg 0 . At the same time, the detection results showed that Hg 2+ , sulfur, S 2− , S − and Fe 2+ had appeared, which demonstrated the probable mercury products, and the H 2 S pre-adsorption and Hg 0 oxidation could be confirmed as well by the different groups of comparative tests. In conclusion, our experimental results are in good agreement with our previous experiments and computational results.
✓ 已验证
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2017
·
IF 3.752
Tiantian Cao,Zijian Zhou,Qian Chen,Zhen Li,Shengming Xu,Jianlong Wang,Minghou Xu,Teresa Bisson,Zhenghe Xu
A novel class of magnetically responsive catalytic sorbents are proposed and synthesized with a potential application to simultaneous removal of Hg 0 and NO at low temperature from the flue gases of coal-fired power plants. The catalytic sorbent consists of magnetite (Fe 3 O 4 ), molecular sieve (HZSM-5), supported silver nanoparticles and catalytically reactive component of V 2 O 5 . Each of these materials provides a unique function for the purpose of capturing mercury, removing NO, and separation from fly ash. After separation from the fly ash, the spent sorbent can be regenerated and reused, leaving an uncontaminated fly ash product. The successful synthesis as designed was confirmed and properties of the catalytic sorbent were characterized by several methods. The synthesized catalytic sorbent was able to completely capture Hg 0 at 150 °C with a capture capacity as high as 32.4 μg·g −1 , while achieving 84% removal of NO at 150 °C. Even at a relatively high space velocity, the catalytic sorbent achieved 97% Hg 0 and 80% NO removal simultaneously, while maintaining a good stability after repetitive regeneration and recycle. The magnetically responsive catalytic composite was shown to be a promising candidate for multi-pollutant emission control from coal-fired power plants.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 46
·69450-69461
·
IF 5.19
Liu Ye,Ma Chenglong,Zhou Jiacheng,Zhu Lin,Cao Limei,Yang Ji
Activated carbon was one of the main adsorptions utilized in elemental mercury (Hg 0 ) removal from coal combustion flue gas. However, the high cost and low physical adsorption efficiency of activated carbon injection (ACI) limited its application. In this study, an ultra-high efficiency (nearly 100%) catalyst sorbent-Se x /Activated carbon (Se x /AC) was synthesized and applied to remove Hg 0 in the simulated flue gas, which exhibited 120 times outstanding adsorption performance versus the conventional activated carbon. The Se x /AC reached 17.98 mg/g Hg 0 adsorption capacity at 160 °C under the pure nitrogen atmosphere. Moreover, it maintained an excellent mercury adsorption tolerance, reaching the efficiency of Hg 0 removal above 85% at the NO and SO 2 conditions in a bench-scale fixed-bed reactor. Characterized by the multiple methods, including BET, XRD, XPS, kinetic and thermodynamic analysis, and the DFT calculation, we demonstrated that the ultrahigh mercury removal performance originated from the activated Se species in Se x /AC. Chemical adsorption plays a dominant role in Hg 0 removal: Selenium anchored on the surface of AC would capture Hg 0 in the flue gas to form an extremely stable substance-HgSe, avoiding subsequent Hg 0 released. Additionally, the oxygen-containing functional groups in AC and the higher BET areas promote the conversion of Hg 0 to HgO. This work provided a novel and highly efficient carbon-based sorbent -Se x /AC to capture the mercury in coal combustion flue gas.
Selenium-modified porous activated carbon and the interface functional group promotes the synergistic effect of physical adsorption and chemical adsorption to promote the adsorption capacity of Hg 0 .
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2016
·
IF 5.31
Yi Xu,Limei Cao,Wei Sun,Ji Yang
A diffusion electrochemical reactor was proposed to remove elemental mercury (Hg 0 ) from coal-fired flue gas. The experiments were carried out in an undivided column reactor with a self-made gas diffusion electrode (GDE) as cathode and Ti/IrO 2 as anode. Hg 0 was oxidized when the simulated gas passed through GDE. It turned out that the removal of Hg 0 in electrochemical process was dominated by electro-generated H 2 O 2 and free radicals on GDE interface or in the electrolyte. Under 70 °C, Hg 0 removal efficiency exceeded 90% after 40 min electrolysis. The effects of operation parameters were investigated and the results demonstrated that voltage, gas flow rate, and initial concentration of Hg 0 had significant influences on Hg 0 removal, especially the reaction temperature, electrolyte concentration and pH. H 2 O 2 and HO in the electrolyte were measured by UV–vis spectrophotometer and electron spin resonance (ESR), respectively. The above results show that electrochemical technique is a promising method for emission control of Hg 0 from coal-fired flue gas.
研究领域:
环境工程
·
电化学
·
空气污染控制
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Hui Liu,Hao Chen,Xiaofeng Xie,Chaofang Li,Fenghua Shen,Pingshan Wang,Kaisong Xiang
Low-temperature gaseous elemental mercury (Hg 0 ) abatement is an objective demand in industrial flue gas treatment . In this work, we proposed a new approach for Hg 0 capture via weak interaction of ionic liquids . Ionic liquids with varied anions (1-butyl-3-methylimidazolium thioacetate ([Bmim][ThAc]), 1-butyl-3-methylimidazolium diethyldithiocarbamate ([Bmim][DTCR]), and 1-butyl-3-methylimidazolium ethylxanthate ([Bmim][EX])) were designed and synthesized. The interaction energies between ionic liquids and elemental mercury were proved to be positively related to mercury removal efficiency, revealing that the electrostatic interaction derived physical adsorption from anions is the dominant factor affecting mercury removal performance. [Bmim][ThAc] with the largest anionic electrostatic interaction energy showed the best mercury abatement performance, achieving a Hg 0 removal efficiency of over 98% and an adsorption capacity of 10.66 mg/g at 50 °C. The influence of temperature and the results of mercury temperature-programmed desorption (Hg-TPD), X-ray photoelectron spectroscopy (XPS) further confirmed that the ionic liquid combines with elemental mercury through physical adsorption. The work provides a new perspective on designing high-efficiency sorbents for mercury removal at low temperature.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Yang Yang,Rui Huang,Wenqing Xu,Jixiang Zhang,Chaoqun Li,Jianfei Song,Tingyu Zhu
ZnS is a promising sorbent in recovering Hg0 from industrial flue gas due to its excellent Hg0 adsorption capacity. However, the internal structure–activity relationship still needs to be further clarified. In this work, ZnS sorbents with different structures were synthesized with the hydrothermal method by tuning the temperature. The samples had significant differences in the crystallinity, morphology, particle size, and sulfur (S) active sites. The results indicated that Hg0 removal performance was determined by the specific surface area and S active sites. ZnS synthesized at low temperatures (80-ZnS and 120-ZnS) had a larger surface area, while the S sites on the high-temperature-synthesized sample (160-ZnS) were more active for Hg0 adsorption. The 160-ZnS sample exhibited a much higher Hg0 adsorption amount per unit surface area. Further characterization revealed that S22– and Sx were the main active sites for Hg0 adsorption. Sx existed in the form of long-chain polysulfur (L-Sx) on 80-ZnS and 120-ZnS, while it exhibited in the form of short-chain polysulfur (S-Sx) on 160-ZnS. L-Sx had negligible adsorption ability, while S-Sx had a high affinity for Hg0. Hg0 can react with S22– and S-Sx, forming α-HgS and β-HgS, respectively. The new insight in this work can provide theoretical guidance for the design and structure optimization of ZnS, facilitating its practical industrial application.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
CATALYSIS COMMUNICATIONS
·
2024
·
IF 3.4
Yu Wang,Bin Zhou,Jingjie Guo,Tao Liu,Yu Yang,Bing Li,Jiaojiao Yang,Yue Peng,Jianjun Chen,Wenzhe Si,Junhua Li
Developing high-performance mercury removal catalysts is essential for addressing atmospheric mercury pollution. Notably, conventional mineral adsorbents are ineffective for high-temperature flue gases (>300 °C). In this study, confinement catalysis was utilized to modify CuMn 2 O 4 . Under the chlorine-free catalytic condition, the temperature window of T 95 was widened by 150 °C (for 50–400 °C) toward high-temperature. Mechanistic studies suggest that nanoconfinement effects significantly improve the catalytic performance. Molecular oxygen adsorption and activation capacity were dramatically enhanced, as demonstrated by NAP-XPS. The plentiful grain boundaries effectively adjust the defect species and electronic structure of the catalysts in favor of Hg 0 catalysis, whereas the porous structure improves the reactant adsorption properties.
研究领域:
环境科学
·
催化
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Jing Yang,Heng-Quan Chen,Fen Qiao,Xifeng Zhu,Tao Wang,Wei-Ping Pan
Engineering metal-based nanoarchitectures and their atomic-scale arrangement is a promising avenue for enhanced mercury adsorbent activities. Interactions between metal single atoms and substrates result in regulated transitions between distinct reaction processes that boost mercury adsorption activity. Herein, a novel sorbent of porous Co 3 O 4 with Palladium atomic dispersed was successfully prepared by one-step pyrolysis of zeolitic imidazolate framework 67 (ZIF-67) precursors. Via engineering single Pd atoms into ZIF-derived Co 3 O 4 (Pd 1 /Co 3 O 4 -ZIF), the strong metal-support interaction (SMSI) activated the reducibility of Co 3+ in porous Co 3 O 4 to efficiently adsorb and oxidize Hg 0 , enhancing its mercury removal efficiency. Specifically, Pd 1 /Co 3 O 4 -ZIF exhibited superior sorption performance for Hg 0 over a broad range of temperatures (30–350 °C) and high gaseous hourly space velocity (about 555,500 hr −1 ) with the average Hg 0 removal efficiency higher than 98%. The strategy of constructing atomic active sites on the surface of porous metal-oxide to convert adsorbed Hg 0 into HgO is a promising approach to solve the problem that Hg 0 in flue gas is challenging to remove. Density functional theory (DFT) calculation further proved that the existence of a single Pd site on the surface of Co 3 O 4 significantly reduced the energy barrier of Hg 0 to HgO at the atomic level. This work contributed to a thorough comprehension of the structural and adsorption properties of the ZIF-derived Co 3 O 4 sorbent engineering with a single atom and enabled the efficient capture of elemental mercury in flue gas by such ZIF-derived sorbent.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Yili Zhang,Yongchun Zhao,Zhuo Xiong,Rihong Xiao,Tian Gao,Pengfei Liu,Jing Liu,Junying Zhang
The application of photocatalytic Hg 0 oxidation under visible light is an up-and-coming method to solve the problem of energy shortage and environmental pollution. In this work, iodine doped Bi 2 MoO 6 nanomaterials were prepared by one-step solvothermal method . The photocatalytic oxidation efficiency was greatly improved by iodine doping from 35.5% to 95.2% in the N 2 + 4% O 2 atmosphere under visible light. The main reason was that iodine doping decreased the band gap of the catalyst, expanded the optical response range and intensity, sped up the separation rate of photoinduced carriers and reduced the recombination rate. In addition, the flue gas components of SO 2 and NO played a promoting role in mercury removal. Iodine doped Bi 2 MoO 6 had good stability and still maintained high mercury removal efficiency after 5 cycles. Density functional theory (DFT) calculations and experiments demonstrated that iodine doping changed the valence band and conduction band of the catalyst, making superoxide ions, hydroxyl radicals and photoinduced hole become the active species of the catalytic reaction .
研究领域:
环境科学
·
材料科学
✓ 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）