SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Yibing Xie,Huihui Wu,Jianfei Luo,Shao Zhang,Langlang Wang,Xueqian Wang,Yixing Ma,Ping Ning
The incorporation of vanadium during the synthesis process induced a spontaneous and complete thermal phase transition from α-Bi 2 O 3 to β-Bi 2 O 3 . This phase transition facilitated the development of intrinsic electric field at the interface between V 2 O 5 and β-Bi 2 O 3 , consequently establishing a novel carrier transfer pathway. As a result, the fabricated V 2 O 5 /β-Bi 2 O 3 heterojunction exhibited an outstanding removal efficiency of over 98 % for gaseous mercury (Hg 0 ) under UV light, and this efficiency of 95.0 % even after 35 h of testing. Introducing vanadium enhanced the light absorption capacity in the ultraviolet region and effectively separated photoinduced charge carriers. As revealed by density functional theory calculations, the photoinduced electron–hole transfer in the V 2 O 5 /β-Bi 2 O 3 heterojunction followed the Z-scheme mechanism. This mechanism significantly contributed to the long-term stability of photocatalytic Hg 0 removal, even when H 2 O and NO were present. This study presents a novel material composited by a thermal phase transition technique, aimed at the highly effective and green removal of Hg 0 in the environment.
研究领域:
环境科学
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材料科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Xin Huang,Zijun Ran,Zhi He,Jingyu Ran
Mercury has a significant impact on environment and is mainly derived from coal-fired power plant. Herein, we report a potential route for efficient removal of Hg 0 via oxidation reactions using Ce-doped LaCoO 3 supported on CeO 2 catalyst. Catalyst characterization results proved that Ce can successfully substitute a desired part of Co into the LaCoO 3 crystal lattice via a sol–gel method. The Hg 0 removal experiments suggest that Hg 0 removal efficiency decreased in the order of La 0.875 Ce 0.125 CoO 3 /CeO 2 > La 0.875 Ce 0.125 CoO 3 > LaCoO 3 . The presence of O 2 provided more active oxygen and resulted in approaching 100% Hg 0 removal efficiency. Introducing H 2 O and sole SO 2 would significantly reduce the Hg 0 removal efficiency as a result of competitive adsorption on the actives sites of the catalyst. On the other hand, SO 2 could reacted with Hg 0 in the presence of O 2 and thereby recover the high Hg 0 removal efficiency and the La 0.875 Ce 0.125 CoO 3 /CeO 2 catalyst presented a good performance towards sulfur resistance. Furthermore, the catalyst still exhibited a high Hg 0 removal efficiency performance after five times consecutive recycles.
研究领域:
环境科学
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催化
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材料科学
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能源工程
✓ 已验证
DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 9
·799
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IF 4
Xuhui Wei,Ruoyang Du,Rushan Zhao,Wenzhi Li,Caihong Jiang,Junwei Wang
The efficient removal of elemental mercury (Hg0) from coal-fired flue gas is a critical challenge in environmental governance. This study proposes utilizing waste fluid catalytic cracking catalyst (WFCC) as the potential support for Hg0catalytic oxidation. After activation (AFCC) via calcination decarbonization, a composite support (AFCC-PG) was fabricated using palygorskite (PG) as a binder. Subsequently, VOxwas loaded onto the support to form the VOx/AFCC-PG catalyst for Hg0removal. Experimental results demonstrate that the VOx/AFCC-PG catalyst achieves >95% Hg0removal efficiency under simulated flue gas conditions (150 °C, GHSV = 6000 h−1) while maintaining excellent stability over 60 h. Furthermore, Hg-TPD and XPS analyses indicate that the synergistic lattice oxygen oxidation–adsorption established between VOxand the AFCC-PG plays a key role in efficient Hg0removal. This study proposes a cost-effective strategy for both the resource utilization of waste catalysts and the control of mercury pollution in coal-fired flue gas.
研究领域:
环境科学
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催化化学
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污染控制
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废弃物资源化
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能源工程
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2021
·
IF 3.605
Wenbo Jia,Chuanmin Chen,Songtao Liu,Yue Cao
In this study, the Hg0 removal characteristics of NaClO2 in limestone slurry were investigated in a bubbling reactor. The effects of slurry conditions (pH, temperature, and Cl– concentration) and flue gas components (NO, SO2, HCl, etc.) on Hg0 removal activity and efficient Hg0 removal duration were explored. X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) were used to characterize the solid products prepared under different conditions. It was found that NaClO2 exhibited superior Hg0 removal activity when both SO2 and NO were present in the flue gas, while the Hg0 removal efficiency reduced significantly in the absence of SO2 and/or NO. The Hg0 removal activity of NaClO2 decreased significantly with the increase of pH value. The slurry temperature had no obvious effect on Hg0 removal activity, while higher temperature could enhance the Hg0 re-emission at a later stage. However, the presence of Cl– in limestone slurry could notably inhibit the Hg0 re-emission. The characterization results showed that the presence of SO2 and NO promoted the formation of HgCl2, Hg(NO3)2, and HgSO4, thus significantly enhancing the Hg0 removal activity of NaClO2 in limestone slurry.
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
CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Yahui Wang,Qihuang Huo,Huijun Chen,Yu Feng,Jiancheng Wang,Sheng Wang,Liping Chang,Weiren Bao
To develop the high value utilization of high organic sulfur coal instead of combustion as well as save the cost of mercury pollution control, we attempted to transmute the inherent sulfur of high organic sulfur coal, in the case of LF coal (which is from Linfen city, China), to active sulfur species for mercury capture by doping metal oxides, and CuO performed best among various metal oxides. The sorbent (or activated sample) prepared from LF coal with doping CuO is labelled LF+Cu-A, around which a series of experiments were conducted. Firstly, the effects of operational conditions, including GHSV (gas hourly space velocity), temperature and flue components, on the mercury capture performance of LF+Cu-A were thoroughly investigated, and results showed that LF+Cu-A had an excellent mercury capture performance. The average mercury capture efficiency is 97.8 % during a two-hour test under N 2 +O 2 +H 2 O+SO 2 +NO atmosphere with GHSV of 240000 h −1 and temperature of 120 °C. Secondly, the experimental data were fitted by four kinetic models, and it is found that the mercury adsorption process under low temperatures (60, 90, 120 °C) and high temperature (150 °C) are in the best agreement with the pseudo-first-order model and the intra-particle diffusion model respectively. Last, the mercury capture mechanisms of LF+Cu-A were revealed by Hg-TPD (Hg-temperature programed desorption) experiment, Raman analysis and XPS (X-ray photoelectron spectrometer) spectra, and it is indicated that the multiple sulfur species and Cu 2+ play roles in the mercury capture process, during which elemental mercury are oxidized to HgS and fixed on the surface of LF+Cu-A.
研究领域:
环境科学
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能源技术
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Wei Zheng,Zequn Yang,Jiefeng Chen,Mingguang Zhang,Hongxiao Zu,Ruiyang Qin,Wenqi Qu,Jianping Yang,Lijian Leng,Hailong Li
Utilization of monolithic mineral sulfide-based sorbent for the fix-bed elemental mercury (Hg 0 ) removal is regarded as a predominant predicament in the field of Hg 0 abatement. In this work, a general and facile route was exploited to establish CuS particles decorated 3D porous Ti 3 C 2 T x MXene aerogel via divalent Cu 2+ cations induced assembly combined with subsequent high-temperature sulfurization treatment, during which, uniform CuS particles were homogeneously anchored throughout the Ti 3 C 2 T x substrate. The obtained 3D CuS/Ti 3 C 2 T x MXene aerogel exhibited satisfactory textural property, hierarchical pore structure and strong interaction between Ti 3 C 2 T x MXene and CuS. Meanwhile, the inherent restacking of Ti 3 C 2 T x MXene nanosheet and serious agglomeration of CuS can also be effectively avoided in the formation of aerogel. Those structural advantages originating from this novel gelation process favorably contributes to satisfactory Hg 0 mass transfer and sufficient utilization of CuS active ligands, which largely strengthens Hg 0 removal performance and broadens the fix-bed application of mineral sulfides. Consequently, the Hg 0 capture capacity and adsorption rate of CuS/Ti 3 C 2 T x MXene aerogel reached 90596.4 g m −3 and 120.64 g m −3 min −1 , respectively, far outbalancing those of the reported in-situ selenized copper foam with excellent Hg 0 removal activity. The impressive Hg 0 sequestration performance is attributed to its relatively large specific surface area, layered pore channel, and highly dispersed CuS particles, largely boosting Hg 0 mass transfer and following sequestration. Moreover, other mineral sulfides/Ti 3 C 2 T x MXene aerogels can also be constructed by just replacing divalent metal cations, which makes the initial effort towards the fix-bed utilization of mineral sulfides-based aerogel for vapor-phase Hg 0 immobilization.
研究领域:
环境科学
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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
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Liyuan Zhang,Shu Yang,Yuekun Lai,Hui Liu,Yiang Fan,Cao Liu,Haiying Wang,Liyuan Chai
Gaseous Hg 0 is one of the most deadly and hard-to-dispose pollutants. The oxidation of Hg 0 is a promising route, but the rational design and synthesis of highly efficient catalysts still remain grand challenges. Herein, CuO@Cu 2 O (or Cu x O) heterostructured nanoparticles uniformly monodispersing on porous carbon monolith were designed and successfully synthesized using oligo( m -phenylenediamine)-Cu 2+ complex as raw material. The Cu x O-carbon catalyst contains ∼28 wt% of Cu. Based on density functional theory calculation, the CuO@Cu 2 O junction interfaces can accelerate the Hg 0 oxidation by significantly reducing the energy barriers of reaction. Only 1 mg of the catalyst can catalyze the oxidation of more than 90 % of Hg 0 with [HCl] = 0.5 ppm, [O 2 ] = 6 vol%, T = 150 °C. The poisoning effect of either SO 2 or H 2 O on the catalysts is weak. Moreover, a long-term test confirmed that the Hg 0 oxidation rate can maintain more than 90 % even in the co-presence of SO 2 (5000 ppm) and H 2 O (10 vol%).
研究领域:
环境催化
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材料化学
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大气污染控制
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纳米材料
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表面科学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2024
·
IF 0
Zheng Yang,Zhang Lin,Wang Xiaocong,Guo Fenghui,Xing Yi,Li Guoliang,Yue Tao
The substantial amount of mercury emissions from coal-fired flue gas causes severe environmental contamination. With the Minamata Convention now officially in force, it is critical to strengthen mercury pollution control. Existing activated carbon injection technologies suffer from poor desulfurization performance and risk secondary-release risks. Therefore, considering the potential industrial application of adsorbents, we selected cost-effective and readily available activated coke (AC) as the carrier in this study. Four metal selenides—copper, iron, manganese, and tin—were loaded onto the AC to overcome the application problems of existing technologies. After 120 min of adsorption, the CuSe/AC exhibited the highest efficiency in removing Hg 0 , surpassing 80% according to the experimental findings. In addition, the optimal adsorption temperature window was 30–120 °C, the maximum adsorption rate was 2.9 × 10 −2 mg·g −1 ·h −1 , and the effectiveness of CuSe/AC in capturing Hg 0 only dropped by 5.2% in the sulfur-containing atmosphere. The physicochemical characterization results indicated that the AC surface had a uniform loading of CuSe with a nanosheet structure resembling polygon and that the Cu-to-Se atomic ratio was close to 1:1. Finally, two possible Hg 0 reaction pathways on CuSe/AC were proposed. Moreover, it was elucidated that the highly selective binding of Hg 0 with ligand-unsaturated Se − was the key factor in achieving high adsorption efficiency and sulfur resistance in the selenium-functionalized AC adsorbent. This finding offers substantial theoretical support for the industrial application of this adsorbent. Graphical Abstract
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
ANALYTICAL CHEMISTRY
·
2015
·
IF 5.636
Li Deng,Yan Li,Xiuping Yan,Jun Xiao,Cheng Ma,Jing Zheng,Shaojun Liu,Ronghua Yang
Methylmercury (CH3Hg+), the common organic source of mercury, is well-known as one of the most toxic compounds that is more toxic than inorganic or elemental mercury. In seabeds, the deposited Hg2+ ions are converted into CH3Hg+ by bacteria, where they are subsequently consumed and bioaccumulated in the tissue of fish, and finally, to enter the human diet, causing severe health problems. Therefore, sensitive and selective detection of bioaccumulation of CH3Hg+ in fish samples is desirable. However, selective assay of CH3Hg+ in the mercury-containing samples has been seriously hampered by the difficulty to distinguish CH3Hg+ from ionic mercury. We report here that metal amalgamation, a natural phenomenon occurring between mercury atoms and certain metal atoms, combining with DNA-protected silver nanoparticles, can be used to detect CH3Hg+ with high sensitivity and superior selectivity over Hg2+ and other heavy metals. In our proposed approach, discrimination between CH3Hg+ and Hg2+ ions was realized by forming Ag/Hg amalgam with a CH3Hg+-specific scaffold. We have found that Ag/Hg amalgam can be formed on a CH3Hg+-specific DNA template between silver atoms and mercury atoms but cannot between silver atoms and CH3Hg+. With a dye-labeled DNA strand, the sensor can detect CH3Hg+ down to the picomolar level, which is >125-fold sensitive over Hg2+. Moreover, the presence of 50-fold Hg2+ and 106-fold other metal ions do not interfere with the CH3Hg+ detection. The results shown herein have important implications for the fast, easy, and selective detection and monitoring of CH3Hg+ in environmental and biological samples.
研究领域:
环境科学
·
分析化学
·
毒理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Sulfur Chemistry
·
2025
·
IF 1.6
Yongpeng Ma,Jianghui Du,Haobing Yan,Chaobin Shi
Molybdenum disulfide (MoS2) is considered a favorable absorbent for removing heavy metals. However, due to its various morphologies, MoS2 exhibits significant differences in its performance for removing mercury from flue gas. In the present study, the flower-like, spherical MoS2 and W-MoS2 were prepared by regulating the interlayer spacing and doping tungsten (W) in MoS2 for removing gaseous mercury (Hg0). The results show that the number of active sulfur sites (S2- and S22-) was critical to the adsorption performance of MoS2 for Hg0. The flower-like MoS2 demonstrated optimum properties below 125°C which attributed to the presence of dominated S2- sites, while spherical MoS2 and W-MoS2 showed a wider application temperature range (up to 175°C) during Hg0 removal which attributed to the unsaturated sulfur S22- and active oxygen. In terms of the mechanism, Hg0 is directly inserted into the Mo-S bond of MoS2 to form a transition state [Hg·Mo]-S, and then the original Mo-S is interrupted to form a new β-Hg-S bond, or combine with surface oxidation to form HgO. The oxygen in the flue gas can supplement the surface active oxygen on the MoS2, which enables the circulation of Mo5+. Hg0 also reacted with S22- to form α-HgS.
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
FUEL
·
2025
·
IF 7.5
Jie Gao,Zijun Ran,Jingyu Ran,Xin Huang,Chuan Ma,Yunlin Shao
The catalysts utilized for low-temperature catalytic oxidation of Hg 0 from flue gas typically suffer from issues related to H 2 O and SO 2 poisoning. This study focused on doping modification of La 0.875 Ce 0.125 CoO 3 perovskite with promoters and conducted a thorough investigation on the H 2 O and SO 2 resistance through characterization and DFT methods. Experimental results demonstrated that the LCeCO/30 wt% ZrO 2 possessed optimal H 2 O and SO 2 resistance. Under high sulfur (1500 ppm SO 2 ) and high humidity (10 % H 2 O(g)) conditions, it maintained approximately 91 % Hg 0 removal efficiency after thermal regeneration cycles. Characterization results indicated that ZrO 2 doping facilitated the formation of three-dimensional macroporous structure and protected active Co 3+ sites on the surface. Based on DFT calculations, the H 2 O poisoning is attributed to competitive adsorption between H 2 O(g) and Hg 0 on the active sites. Also, the SO 2 poisoning occurs due to competitive adsorption of SO 2 and the toxicity of sulfates to the surface active sites. Meanwhile, ZrO 2 doping can lower the adsorption energies of H 2 O(g) and SO 2 by modifying their adsorption configuration, thus weakening the competitive adsorption of H 2 O(g) and SO 2 with Hg 0 . Overall, LCeCO/ZrO 2 is a promising Hg 0 removal catalyst with superior H 2 O and SO 2 resistance.
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
ENERGY & FUELS
·
2021
·
IF 3.605
Jianwen Guo,Jiang Wu,Yu Guan,Jianmin Wang,Qizhen Liu,Xu Mao,Xuemei Qi,Ping He,Huaning Wang
A Z-scheme heterojunction polyhedral-shaped BiOIO3/MIL-53(Fe) photocatalyst is prepared by a solvothermal method. The samples are characterized by XRD, XPS, SEM, TEM, FT-IR, UV–vis, PL, and other material characterization analysis methods. The photocatalytic performance of photocatalysts is studied for removal of vapor-phase mercury (Hg0) under visible-light irradiation. The results suggest that the Hg0 removal efficiency of the BiOIO3/MIL-53(Fe) composite is significantly improved compared with that of MIL-53(Fe). When the molar ratio of BiOIO3 and MIL-53(Fe) is 2:1, the BiOIO3/MIL-53(Fe) composite photocatalyst exhibits the best Hg0 removal efficiency, reaching 74.19%. BiOIO3 and MIL-53(Fe) form a Z-scheme heterojunction with a suitable energy band structure, which results in the effective separation of photoinduced electron–hole pairs and delays their recombination. Finally, the photocatalytic oxidation mechanism of Hg0 by the BiOIO3/MIL-53(Fe) composite is proposed, which paves the way for the study of the built-in electric field and electron transport channels between binary photocatalyst materials.
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
危险品化学品经营许可证（带存储）