FUEL
·
2017
·
IF 4.601
Dongjing Liu,Weiguo Zhou,Jiang Wu
CuO-based and MnO x -based sorbents modified with Ce and La using sol-gel method, were employed for elemental mercury removal at 120–240 °C. The Hg 0 removal activity of Mn 2 O 3 /ZSM-5 can be significantly enhanced by doping 50 at.% Ce or 10 at.% La, the Hg 0 removal efficiency increased by 94% and 71%, respectively. The Hg 0 removal ability of CuO/ZSM-5 subtly improved by addition of 50 at.% Ce or 10 at.% La, the Hg 0 removal efficiency ascended only by 6% and 18%, respectively. The XPS results revealed that Hg 0 transformed to HgO, and CuO (or Mn 2 O 3 ) was reduced to Cu 2 O (or Mn 3 O 4 ), which is in agreement with Mars-Maessen mechanism.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
FUEL
·
2017
·
IF 4.601
Shaojian Jiang,Xi Liu,Hailong Li,Jun Wang,Zequn Yang,Haoyi Peng,Kaimin Shih
Elemental mercury (Hg 0 ) oxidation over a low-temperature La 2 O 3 -TiO 2 (LaTi) catalyst through a fixed-bed reactor system is reported here. Despite the presence of oxygen (O 2 ), Hg 0 was not effectively oxidized by either hydrogen chloride (HCl) or nitrogen oxide (NO). However, Hg 0 oxidation over the LaTi catalyst was greatly improved when both HCl and NO were present in the simulated flue gas. Several methods, including X-ray photoelectron spectroscopy (XPS), diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy, and temperature-programmed decomposition (TPD), were used to study the inherent mechanisms involved in the Hg 0 oxidation by HCl and NO. The results indicated that the combined presence of HCl and NO exhibited great synergy for Hg 0 catalytic oxidation over the LaTi catalyst. The reaction mechanism is proposed as follows: 1) NO was adsorbed and oxidized on the catalyst surface, forming NO 2 ; 2) the reactive NO 2 then oxidized gas phase Hg 0 to mostly HgO, and; 3) HgO reacted with gas phase HCl to produce HgCl 2 , which escaped from the catalyst’s surface. Differing from previously proposed mechanisms, La 2 O 3 was first studied as an active substance in Hg 0 oxidation. These findings are beneficial for those seeking economical and efficient Hg 0 oxidation catalysts for coal-fired power plants.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
Catalysts
·
2020
·Vol. 10
·期 1
·72
·
IF 3.52
Xiaopeng Zhang,Xiangkai Han,Chengfeng Li,Xinxin Song,Hongda Zhu,Junjiang Bao,Ning Zhang,Gaohong He
Sorbent of αMnO2nanorods coating TiO2shell (denoted as αMnO2-NR@TiO2) was prepared to investigate the elemental mercury (Hg0) removal performance in the presence of SO2. Due the core-shell structure, αMnO2-NR@TiO2has a better SO2resistance when compared to αMnO2nanorods (denoted as αMnO2-NR). Kinetic studies have shown that both the sorption rates of αMnO2-NR and αMnO2-NR@TiO2, which can be described by pseudo second-order models and SO2treatment, did not change the kinetic models for both the two catalysts. In contrast, X-ray photoelectron spectroscopy (XPS) results showed that, after reaction in the presence of SO2, S concentration on αMnO2-NR@TiO2surface is lower than on αMnO2-NR surface, which demonstrated that TiO2shell could effectively inhibit the SO2diffusion onto MnO2surface. Thermogravimetry-differential thermosgravimetry (TG-DTG) results further pointed that SO2mainly react with TiO2forming Ti(SO4)O in αMnO2-NR@TiO2, which will protect Mn from being deactivated by SO2. These results were the reason for the better SO2resistance of αMnO2-NR@TiO2.Keywords:core-shell structure;αMnO2nanorods;elemental mercury removal;SO2resistance
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
产品关联
DOI
高影响因子
Journal of Environmental Sciences
·
2020
·
IF 4.302
Renjun Li,Yanan Zhou,Xueqian Wang,Langlang Wang,Ping Ning,Lei Tao,Jun Cai
La 2 O 3 /Bi 2 O 3 photocatalysts were prepared by impregnation of Bi 2 O 3 with an aqueous solution of lanthanum precursor followed by calcination at different temperatures. The composite materials were used for the first time for the photocatalytic removal of Hg 0 from a simulated flue gas under UV light irradiation. The results showed that the sample containing 6 wt.% La 2 O 3 and calcined at 500°C has the highest dispersion of the active sites, which was promoted by the strong interaction with the support (i.e., the formation of Bi-O-La species). Since they are fully accessible on the surface, the material also exhibits excellent optical properties while the heterojunction formed in La 2 O 3 /Bi 2 O 3 promotes the separation and migration of photoelectron-hole pairs and thus Hg 0 oxidation efficiency is enhanced. The effects of the various factors (e.g., the reaction temperature and composition of the simulated flue gas (i.e., O 2 , NO, H 2 O, and SO 2 )) on the efficiency of the Hg 0 photocatalytic oxidation were investigated. The results demonstrated that O 2 and SO 2 enhanced the efficiency of the reaction while the reaction temperature, NO, and H 2 O had an inhibitory effect.
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
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2016
·
IF 5.393
Hailong Li,Lei Zhu,Jun Wang,Liqing Li,Kaimin Shih
The surface area of zinc sulfide (ZnS) was successfully enlarged using nanostructure particles synthesized by a liquid-phase precipitation method. The ZnS with the highest surface area (named Nano-ZnS) of 196.1 m2·g–1 was then used to remove gas-phase elemental mercury (Hg0) from simulated coal combustion fuel gas at relatively high temperatures (140 to 260 °C). The Nano-ZnS exhibited far greater Hg0 adsorption capacity than the conventional bulk ZnS sorbent due to the abundance of surface sulfur sites, which have a high binding affinity for Hg0. Hg0 was first physically adsorbed on the sorbent surface and then reacted with the adjacent surface sulfur to form the most stable mercury compound, HgS, which was confirmed by X-ray photoelectron spectroscopy analysis and a temperature-programmed desorption test. At the optimal temperature of 180 °C, the equilibrium Hg0 adsorption capacity of the Nano-ZnS (inlet Hg0 concentration of 65.0 μg·m–3) was greater than 497.84 μg·g–1. Compared with several commercial activated carbons used exclusively for gas-phase mercury removal, the Nano-ZnS was superior in both Hg0 adsorption capacity and adsorption rate. With this excellent Hg0 removal performance, noncarbon Nano-ZnS may prove to be an advantageous alternative to activated carbon for Hg0 removal in power plants equipped with particulate matter control devices, while also offering a means of reusing fly ash as a valuable resource, for example as a concrete additive.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2015
·
IF 3.512
Jiang Wu,Xian Li,Jianxing Ren,Xuemei Qi,Ping He,Bu Ni,Chong Zhang,Chengzhen Hu,Jun Zhou
TiO 2 hollow sphere was synthesized by hydrothermal method using trifluoroacetic acid (TFA) and Ti(SO 4 ) 2 as raw materials, and it was applied to photocatalytic oxidization of elemental mercury (Hg 0 ) in the simulated flue gas. The prepared samples were well characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), UV–vis diffuse reflectance spectra (UV-vis DRS) and nitrogen adsorption/desorption. The results showed that only anatase phase TiO 2 hollow sphere was obtained. The average diameter of TiO 2 hollow spheres was about 800 nm and the shell thickness was about 200–400 nm. When M , the molar ratio of TFA to Ti(SO 4 ) 2 , was higher than a certain value, the photocatalytic activity of prepared TiO 2 hollow spheres began to reduce. When M = 2, addition TFA content was the best quantity, which got the best TiO 2 hollow spheres and provided the most appropriate F − decomposed from TFA during the sample preparation, which was helpful to its photocatalytic ability. In the experimental temperature range, the photocatalytic oxidation efficiency decreased with the increasing of reaction temperature, and the intensity of UV irradiation had an important effect on the photocatalytic reaction. When UV irradiation intensity was 303.45 μW cm −2 and reaction temperature was 55 °C, TiO 2 hollow sphere sample prepared at M = 2 had the highest photocatalytic ability and the mercury removal efficiency reached up to 82.75%.
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
Nature Communications
·
2024
·Vol. 15
·期 1
·1-15
·
IF 14.7
Li Hailong,Meng Fanyue,Zhu Penglin,Zu Hongxiao,Yang Zequn,Qu Wenqi,Yang Jianping
Highly efficient decontamination of elemental mercury (Hg 0 ) remains an enormous challenge for public health and ecosystem protection. The artificial conversion of Hg 0 into mercury chalcogenides could achieve Hg 0 detoxification and close the global mercury cycle. Herein, taking inspiration from the bio-detoxification of mercury, in which selenium preferentially converts mercury from sulfoproteins to HgSe, we propose a biomimetic approach to enhance the conversion of Hg 0 into mercury chalcogenides. In this proof-of-concept design, we use sulfur-rich polyphenylene sulfide (PPS) as the Hg 0 transporter. The relatively stable, sulfur-linked aromatic rings result in weak adsorption of Hg 0 on the PPS rather than the formation of metastable HgS. The weakly adsorbed mercury subsequently migrates to the adjacent selenium sites for permanent immobilization. The sulfur-selenium pair affords an unprecedented Hg 0 adsorption capacity and uptake rate of 1621.9 mg g −1 and 1005.6 μg g −1 min −1 , respectively, which are the highest recorded values among various benchmark materials. This work presents an intriguing concept for preparing Hg 0 adsorbents and could pave the way for the biomimetic remediation of diverse pollutants.
研究领域:
环境科学
·
材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hailong Li,Weizhen He,Wei Zheng,Zequn Yang,Yingchao Hu,Wenqi Qu
The limited adsorption capacity of commercialized sorbents towards elemental mercury (Hg 0 ) remains a major challenge facing their extensive applications under the regulation of the Minamata Convention. Metal selenides were recently found to be promising alternatives to commercialized sorbents for capturing Hg 0 from industrial flue gas due to the high affinity between Hg 0 and selenide. In metal selenides, under-coordinated selenide sites play critical roles in oxidation and subsequent immobilization of Hg 0 , while there is still no simple way to increase the abundance of under-coordinated selenide in metal selenides under ambient conditions. In this work, an effective and facile precipitation pathway was proposed to prepare amorphous cobalt selenide (a-CoSe 2 ) with under-coordinated selenide enriched surface under ambient conditions. The a-CoSe 2 as synthesized achieved outstanding Hg 0 uptake capacity and adsorption rate (534.2 mg g −1 and 483.1 μg g −1 min −1 ), far surpassing those of crystalline cobalt selenide (c-CoSe 2 ) by magnitudes. The characteristic results demonstrated that the under-coordinated selenide enriched nature of a-CoSe 2 is the principal reason causing the significant performance improvement, which is fully in line with our hypothesis and purpose. This work not only proposes a potential sorbent for efficient Hg 0 sequestration from industrial flue gas but also inspires the further development of synthesis strategies for amorphous materials.
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
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Yulan Zheng,Peng Cheng,Zikuo Li,Chuhao Fan,Jinchao Wen,Yue Yu,Li Jia
To achieve the efficient removal of gaseous elemental mercury in coal-fired flue gas, the study successfully prepared the isostructural bimetallic MOFs-based biochar composite by introducing the transition metal Fe into the UiO-66 by solvothermal method and using in-situ growth method for structural design. In addition, the effect of doping the secondary metal Fe and biochar on the Hg 0 removal performance and the corresponding quantitative correlation mechanism was established. The results showed that the overall mercury removal performance of the samples after Fe modification was improved. The optimal Fe loading ratio was 10 %, which corresponded to the adsorption capacity of 127.65 μg·g −1 . The biochar promoted the electron transmission and transfer of the overall reaction system by exerting the carrier effect. The 10 %Fe-UiO-66@20 %BC composite showed the best Hg 0 removal performance, with the corresponding adsorption capacity of 150.74 μg·g −1 . Fe 3+ , lattice oxygen, and chemisorbed oxygen jointly participated in the oxidation process of Hg 0 and finally oxidized Hg 0 to HgO.
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
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Hui Wang,Wangsheng Yu,Xu Peng,Zewen Chen,Shengji Wu,Qinqin Yu,Wei Yang,Jie Zhou
In the present work, highly efficient catalytic adsorbents for Hg 0 removal in both oxygen-rich and deficient atmosphere are developed based on an “adaption” strategy. Firstly, a series of simplified SiO 2 -based catalytic adsorbents are prepared as model catalysts to gain a deeper insight into the mechanism of the catalytic Hg 0 removal process. It is found that for the effective Hg 0 removal, the catalytic adsorbent should possess an “assembling” structure involving both Hg 0 and oxygen activation sites. An “adaption” strategy is thus implemented for the devise of the catalytic adsorbent, including the functional adaption of different active sites for the reactants and the synergistic function of different active sites. Accordingly, high-efficiency catalytic adsorbent with strong redox property is developed for oxygen-rich atmosphere, while the catalytic adsorbent with high oxygen storage/release property is developed for oxygen-deficient conditions. Moreover, regeneration investigation indicates that the activities of spent catalytic adsorbents are almost fully recovered through the temperature programmed decomposition and desorption (TPDD) process. It is believed that the present “adaption” strategy for catalyst design has guiding significance for the rational and controllable construction of catalysts for other catalytic processes.
研究领域:
环境催化
·
大气污染控制
·
材料化学
·
表面科学
·
化学工程
·
环境功能材料
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jianping Yang,Xingyue Zhou,Wei Zheng,Penglin Zhu,Fanyue Meng,Zequn Yang,Wenqi Qu,Hailong Li
Efficiently removing elemental mercury (Hg 0 ) from natural gas is a serious task to both equipment safety and ecosystem. The granulation of adsorbent powder is required to reduce pressure loss and adsorbent elutriation from a fixed-bed demercuration system. Herein, urea modified CuO (Urea/CuO) pellets were developed for Hg 0 adsorption from natural gas with H 2 S. The characterization results show that the addition of urea accelerated the formation of pore structure and surface oxygen, thus enhancing the Hg 0 adsorption performance of CuO pellets. The Urea/CuO pellets with 20 % urea additive amount exhibited 93 % Hg 0 removal efficiency under the existence of 500 ppm H 2 S and a gaseous hourly space velocity of 1.21 × 10 5 h −1 . H 2 S was essential to in-situ convert Urea/CuO pellets into a highly active Hg 0 adsorbent. With the increase of H 2 S concentration from 0 to 1000 ppm, the Hg 0 removal efficiency was raised from 34 % to 93 %. Urea/CuO pellets performed well for Hg 0 adsorption at 10–50 °C, which was the representative temperature window of natural gas processing. The Hg 0 adsorption capacity and uptake rate of Urea/CuO with 500 ppm H 2 S reached as high as 27.06 mg·g −1 and 2.44 μg·g −1 ·min −1 , which largely exceeded those of commercial activated carbons specialized for Hg 0 adsorption as well as typical granulated Hg 0 adsorbents reported in previous literature. The existence of H 2 S in natural gas in-situ converted CuO into CuS. The S 2 2− on the formed CuS could act as active sites for Hg 0 adsorption, in which gaseous Hg 0 was captured as stable mercury sulfide (HgS). The deactivated adsorbent could be regenerated and reused by thermally decomposing HgS and replenishing the consumed surface oxygen and the sintering surface. With these advantages, the developed Urea/CuO pellets appears to be a promising Hg 0 adsorbent from natural gas with H 2 S.
研究领域:
环境工程
·
材料科学
·
化学工程
·
气体净化
·
污染控制
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2019
·Vol. 29
·期 17
·1807191
·
IF 15.621
Zequn Yang,Hailong Li,Jianping Yang,Shihao Feng,Xi Liu,Jiexia Zhao,Wenqi Qu,Pu Li,Yong Feng,Po-Heng Lee,Kaimin Shih
A key challenge in elemental mercury (Hg 0 ) decontamination from flue gas lies in the design of a sorbent with abundant reactive adsorption sites that exhibit high affinity toward Hg 0 to simultaneously achieve rapid capture and large capacity. Herein, zeolitic imidazolate framework-8 (ZIF-8) supported copper selenide (CuSe) nanocomposites are synthesized by a newly designed two-step surfactant-assisted method. The as-prepared CuSe/ZIF-8 with CuSe to ZIF-8 mass ratio of 80% (0.8NC-ZIF) exhibits unparalleled performance toward Hg 0 adsorption with equilibrium capacity and average rate reaching 309.8 mg g −1 and 105.3 µg g −1 min −1 , respectively, surpassing all reported metal sulfides and traditional activated-carbon-based sorbents. The impressive performance of 0.8NC-ZIF for Hg 0 immobilization is primarily attributed to the adequate exposure of the Se-terminated sites with high affinity toward Hg 0 resulted from the layered structure of CuSe. The adsorbed mercury selenide exhibits even higher stability than the most stable natural mercury ore—that is, mercury sulfide—hence minimizing its environmental impact when the CuSe/ZIF-8 sorbent is dumped. This work provides a new mindset for future design of sorbents for efficient Hg 0 capture from industrial flue gas. The results also justify the candidature of CuSe/ZIF to be applicable for mercury pollution remediation in real-world conditions.
研究领域:
环境科学
·
材料科学
·
化学工程
·
污染控制
✓ 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）