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学者姓名：郑勇
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Abstract ：
Selective adsorption of sulfur dioxide (SO2) is an important clean technology for purification of exhaust gas from fossil fuel combustion. The widely applied zeolite-based adsorbents interact with SO2 through weakly physical adsorption, resulting in low adsorption capacity and selectivity for SO2. Herein, a facile strategy that combines improving the textural property of zeolite and optimizing adsorption sites is developed for efficient and stable SO2 adsorption. The micro-mesoporous silica sphere (MS) with high specific surface area and well-defined pore structure is obtained through a micelle expander assisted soft-template method, which can facilitate the dispersion and exposure of designed adsorption sites- methylated polyethyleneimine (mPEI). Since the Lewis basic sites of N in mPEI can strongly interact with the pi-receptor SO2, and the tertiary amine groups exhibit a weak attraction for CO2, the optimized MS supported mPEI adsorbent exhibits remarkable SO2 adsorption performance (7.5 mmol/g), exceptionally high SO2/N2 selectivity (16673) and SO2/CO2 selectivity (551). Moreover, it presents an outstanding stability in the adsorption-regeneration test. This work sheds light on the design of high-performance organic-solid composite adsorbent for selective capture of SO2.
Keyword ：
Adsorption Adsorption Micro-mesoporous silica sphere Micro-mesoporous silica sphere Polytertiary amine Polytertiary amine Selective desulfurization Selective desulfurization SO 2 capture SO 2 capture
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| GB/T 7714 | Zhang, Qiongdan , Wei, Jixiang , Gao, Changbo et al. Highly selective capture of SO2 with supported micro-mesoporous silica sphere from CO2-rich environment [J]. | JOURNAL OF CLEANER PRODUCTION , 2024 , 436 . |
| MLA | Zhang, Qiongdan et al. "Highly selective capture of SO2 with supported micro-mesoporous silica sphere from CO2-rich environment" . | JOURNAL OF CLEANER PRODUCTION 436 (2024) . |
| APA | Zhang, Qiongdan , Wei, Jixiang , Gao, Changbo , Zheng, Yong , Xiao, Yihong , Liu, Fujian et al. Highly selective capture of SO2 with supported micro-mesoporous silica sphere from CO2-rich environment . | JOURNAL OF CLEANER PRODUCTION , 2024 , 436 . |
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Ordered mesoporous carbon@silica hybrid frameworks with high nitrogen content and good stabilities show great significance to improve their functionalities. Herein, we report novel nitrogen-doped (3.51 - 4.62 wt%) and ordered mesoporous carbon@silica frameworks (N-OMC@SiO2) with reinforced nitrogen stability. The NOMC@SiO2 were designed from tricomponent direct co-assembly between block copolymer template and mixed precursors containing urea and tetramethoxysilane without using additional solvent. The N-OMC@SiO2 have large BET surface areas (444.3 - 674.9 m2/g), uniform mesoporous channels (5.8 - 10.9 nm) with well-defined hexagonal symmetry, and stable carbon@silica "reinforced concrete" framework that can be transformed into carbon@silicon by controllable reduction. The nitrogen sites were firmly embedded into their frameworks via the formation of Si-N bonding. Thus, the resulted N-OMC@SiO2 exhibit multi-functionalities and enhanced recyclability in acid waste gas capture and gaseous sulfides catalytic utilization, better than many reported porous adsorbents and catalysts. This study may help develop stable and efficient N-OMCs nanocomposites for acidic gas selective removal.
Keyword ：
Acid gas selective capture Acid gas selective capture Carbon@silica composites Carbon@silica composites Gaseous sulfides elimination Gaseous sulfides elimination Nitrogen -doping Nitrogen -doping Ordered mesoporosity Ordered mesoporosity Solvent -free synthesis Solvent -free synthesis
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| GB/T 7714 | Kan, Xun , Liu, Zihao , Sun, Yafei et al. Tricomponent direct co-assembly to nitrogen-doped, ordered mesoporous carbon@silica frameworks with enhanced nitrogen stability and multi-functionalities [J]. | CHEMICAL ENGINEERING SCIENCE , 2024 , 292 . |
| MLA | Kan, Xun et al. "Tricomponent direct co-assembly to nitrogen-doped, ordered mesoporous carbon@silica frameworks with enhanced nitrogen stability and multi-functionalities" . | CHEMICAL ENGINEERING SCIENCE 292 (2024) . |
| APA | Kan, Xun , Liu, Zihao , Sun, Yafei , Zhong, Shouchao , Zheng, Yong , Liang, Shijing et al. Tricomponent direct co-assembly to nitrogen-doped, ordered mesoporous carbon@silica frameworks with enhanced nitrogen stability and multi-functionalities . | CHEMICAL ENGINEERING SCIENCE , 2024 , 292 . |
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The amine -based materials pose high potential for the adsorption of sulfur dioxide (SO 2 ). This work is aimed at modulating the morphologies of SBA -15 adsorbents by controlling the precursor self -assembly processes, for the sake of optimizing the utilization efficiency of amine species in the polytertiary amine (PTA)-functionalized SBA15. It results that worm -like SBA -15 (WLS) material shows a better particle aspect ratio and well-defined pore structure, which helps to optimize the adsorption sites invoked by the preferable dispersion and exposure of PTA, thus amplifying the chemisorption of SO 2 on the adsorbent. Consequently, the functionalized WLS-PTA adsorbent exhibits remarkable SO 2 adsorption performance (15.43 mmol/g), exceptionally high selectivities of SO 2 /N 2 (27522) and SO 2 /CO 2 (652). Surprisingly, the desulfurization capacity can be further enhanced by the positive effect of the water vapor co -fed. It is unveiled that the whole SO 2 adsorption process mainly follows the dual site Langmuir-Freundlich isotherm model and Bangham model. This work sheds light on the design of polymer -solid composite adsorbents for selective capture of SO 2 .
Keyword ：
Mesoporous SBA-15 Mesoporous SBA-15 Polytertiary amine Polytertiary amine Selective desulfurization Selective desulfurization SO2 adsorption SO2 adsorption Solid amine adsorbent Solid amine adsorbent
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| GB/T 7714 | Zhang, Qiongdan , Lei, Yuanyi , Ye, Ming et al. Facilely tuning the morphologies of tertiary amine-functionalized SBA-15 for optimizing selective SO 2 capture [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 487 . |
| MLA | Zhang, Qiongdan et al. "Facilely tuning the morphologies of tertiary amine-functionalized SBA-15 for optimizing selective SO 2 capture" . | CHEMICAL ENGINEERING JOURNAL 487 (2024) . |
| APA | Zhang, Qiongdan , Lei, Yuanyi , Ye, Ming , Wang, Heng , Zheng, Yong , Xiao, Yihong et al. Facilely tuning the morphologies of tertiary amine-functionalized SBA-15 for optimizing selective SO 2 capture . | CHEMICAL ENGINEERING JOURNAL , 2024 , 487 . |
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NH3 reversible adsorption and separation show great significance during its production and utilization, tradi-tional adsorbents show either complex synthetic procedures or unsatisfied separation precision. We report here a class of sulfonic group functionalized and ordered mesoporous silica superacids (OMS-SO3H-xs) via enhanced host-guest assembly between copolymer templates and silica precursors without additional solvent. The OMS-SO3H-xs have large surface areas (463.7-910.5 m2/g), abundant micropores tandem well-ordered mesopores, high concentration of -SO3H (2.5 mmol/g) with extremely-high acid strength. Consequently, the OMS-SO3H-xs exhibit ultra-high precision for NH3 reversible adsorption and separation, giving high NH3 capacity (9.0 & 7.6 mmol/g at 25 & 50 degrees C and 1.0 bar) with extraordinary NH3/N2 (0.1/0.9) Ideal Adsorption Solution Theory (IAST) selectivities (1200 & 2235). The room temperature saturated breakthrough NH3 capacities of OMS-SO3H-xs were up to 3.38 mmol/g (3.0v%NH3/24.75v%N2/72.25v%H2), which can be well-maintained after 8th cycling without attenuation. The above features found in the OMS-SO3H-xs were resulted from their high density of -SO3H superacid sites those were homogeneously anchored into the ordered mesoporosity, which not only enhances their interaction with NH3, but also achieves the controllable NH3 interaction and transportation inside the mesochannels.
Keyword ：
Enahnced host-guest assembly Enahnced host-guest assembly NH 3 controllable transportation NH 3 controllable transportation Ordered mesopores Ordered mesopores Reversible adsorption and separation Reversible adsorption and separation Solid superacids Solid superacids
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| GB/T 7714 | Zhang, Wentao , Liu, Fengqing , Kan, Xun et al. Developing ordered mesoporous silica superacids for high-precision adsorption and separation of ammonia [J]. | CHEMICAL ENGINEERING JOURNAL , 2023 , 457 . |
| MLA | Zhang, Wentao et al. "Developing ordered mesoporous silica superacids for high-precision adsorption and separation of ammonia" . | CHEMICAL ENGINEERING JOURNAL 457 (2023) . |
| APA | Zhang, Wentao , Liu, Fengqing , Kan, Xun , Zheng, Yong , Zheng, Anmin , Liu, Fujian et al. Developing ordered mesoporous silica superacids for high-precision adsorption and separation of ammonia . | CHEMICAL ENGINEERING JOURNAL , 2023 , 457 . |
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Selective catalytic oxidation of H2S into elemental sulfur has been recognized as the optimal route for H2S reutilization, but traditional metal catalysts show poor sulfur resistance. Herein, we report a solvent-free route for designing nitrogen and defects co-doped, ordered mesoporous carbons (ND-OMCs) from co-assembly of block copolymer template with nitrogen-containing oligomers and silica defects directing agent. Through thermal curing, carbonization and etching of silica, the microporosity tandem ordered mesopores, abundant nitrogen sites (6.13 wt%) and structural defects were introduced into ND-OMCs. The ND-OMCs were successfully applied as efficient and long-lived metal-free catalysts for H2S selective oxidation to sulfur, giving nearly 100 % H2S conversion and sulfur selectivity at only 150 degrees C. Their remark-able activities of ND-OMCs can be well-maintained over 157 h of continuous reaction, exhibiting the sul-fur capacity as high as 3295 mg/g, which were much better than mostly desulfurizes such as commercial Fe2O3, g-C3N4, and nitrogen-containing, ordered mesoporous carbons.(c) 2023 Elsevier Ltd. All rights reserved.
Keyword ：
H2S catalytic reutilization H2S catalytic reutilization Nitrogen-doped porous carbon Nitrogen-doped porous carbon Ordered mesoporosity Ordered mesoporosity Structural defects Structural defects Sustainable design Sustainable design
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| GB/T 7714 | Kan, Xun , Song, Feiyu , Zhang, Guanqing et al. Sustainable design of co-doped ordered mesoporous carbons as efficient and long-lived catalysts for H2S reutilization [J]. | CHEMICAL ENGINEERING SCIENCE , 2023 , 269 . |
| MLA | Kan, Xun et al. "Sustainable design of co-doped ordered mesoporous carbons as efficient and long-lived catalysts for H2S reutilization" . | CHEMICAL ENGINEERING SCIENCE 269 (2023) . |
| APA | Kan, Xun , Song, Feiyu , Zhang, Guanqing , Zheng, Yong , Zhu, Qiliang , Liu, Fujian et al. Sustainable design of co-doped ordered mesoporous carbons as efficient and long-lived catalysts for H2S reutilization . | CHEMICAL ENGINEERING SCIENCE , 2023 , 269 . |
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Abstract ：
作为钢铁生产大国，我国的钢铁年产量已超过10.3亿吨，位居世界第一位。高炉煤气/转炉煤气是以煤炭为原料的高炉炼铁行业的副产品，其年产量高达1.8万亿立方米，实现对高炉煤气/转炉煤气的清洁高效再利用是国家的重大需求。目前，钢铁企业实现高炉煤气及转炉煤气的综合利用主要包括：一种是直接给锅炉、热风炉和加热炉等作为燃料使用；另一种是利用高炉煤气的余压发电，再将发电用后的高炉煤气作为燃料供锅炉、热风炉和加热炉等使用。随着我国能源结构及环保要求的不断完善，综合利用高炉煤气/转炉煤气并按照工业合成氨的原料工艺要求进行净化、配比后制取绿氢，并作为原料用于合成氨，不仅能够满足区域经济发展对绿色合成氨产能的需求，还能够实现高炉煤气/转炉煤气资源重整，促进区域经济绿色发展，符合当前国家对合成氨及钢铁行业提出的节能减排的要求。基于此，本综述对高炉煤气/转炉煤气低碳高效合成氨工艺流程及其优势进行系统分析与展望。
Keyword ：
低碳高效 低碳高效 合成氨工艺流程 合成氨工艺流程 转炉煤气 转炉煤气 高炉煤气 高炉煤气
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| GB/T 7714 | 刘福建 , 郑勇 , 曹彦宁 et al. 高炉煤气/转炉煤气低碳高效合成氨工艺流程 [J]. | 过程工程学报 , 2023 , 23 (03) : 350-358 . |
| MLA | 刘福建 et al. "高炉煤气/转炉煤气低碳高效合成氨工艺流程" . | 过程工程学报 23 . 03 (2023) : 350-358 . |
| APA | 刘福建 , 郑勇 , 曹彦宁 , 江莉龙 . 高炉煤气/转炉煤气低碳高效合成氨工艺流程 . | 过程工程学报 , 2023 , 23 (03) , 350-358 . |
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As a major steel producer, the annual output of steel in China has reached 1.03 billion tons, ranking the highest amount over the world. Blast furnace gas/converter gas is the by-products of the blast furnace ironmaking industry, and its annual output is as high as ~1.8 trillion m3. Therefore, the realizing the clean and efficient utilization of blast furnace gas/converter gas is a major demand for the sustainable development. At present, the integrated utilization of blast furnace gas and converter gas by iron and steel companies mainly includes: one part is directly used as fuel for boilers, hot blast stoves, heating furnaces, etc.; The other part is to use the residual pressure of blast furnace gas to generate electricity, and then use the blast furnace gas as fuel for boilers, hot blast furnaces, and heating furnaces. With the continuous improvement of energy structure and environmental protection requirements in China, the integrated utilization of blast furnace gas/converter gas, purification and proportioning according to the raw material process requirements of industrial synthetic ammonia to produce green hydrogen, which is used as the raw feedstocks for synthetic ammonia. It can not only meet the demand of regional economic development for green synthetic ammonia production, but also realize the reorganization of blast furnace gas/converter gas resources. As a result, the new technique promotes the green development of the regional economy, which meets the current national requirements for energy saving and emission reduction for ammonia synthesis and the steel industry. Based on this, this review systematically analyzes and forecasts the low-carbon and high-efficiency ammonia synthesis process from blast furnace gas/converter gas and demonstrates the advantages of the developed technique. Key learning points: (1) The origin and development trend of synthetic ammonia process are summarized. (2) The development status of ammonia synthesis process with blast furnace gas/converter gas is summarized. (3) The characteristics, significance, and development direction of the ammonia synthesis process with blast furnace gas/converter gas are summarized and proposed. © 2023 Science Press. All rights reserved.
Keyword ：
blast furnace gas blast furnace gas converter gas converter gas high-efficiency high-efficiency low-carbon low-carbon synthetic ammonia process flow synthetic ammonia process flow
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| GB/T 7714 | Fujian, L. , Yong, Z. , Yanning, C. et al. Low-carbon and high-efficiency ammonia synthesis process from blast furnace gas/converter gas; [高炉煤气/转炉煤气低碳高效合成氨工艺流程] [J]. | The Chinese Journal of Process Engineering , 2023 , 23 (3) : 350-358 . |
| MLA | Fujian, L. et al. "Low-carbon and high-efficiency ammonia synthesis process from blast furnace gas/converter gas; [高炉煤气/转炉煤气低碳高效合成氨工艺流程]" . | The Chinese Journal of Process Engineering 23 . 3 (2023) : 350-358 . |
| APA | Fujian, L. , Yong, Z. , Yanning, C. , Lilong, J. . Low-carbon and high-efficiency ammonia synthesis process from blast furnace gas/converter gas; [高炉煤气/转炉煤气低碳高效合成氨工艺流程] . | The Chinese Journal of Process Engineering , 2023 , 23 (3) , 350-358 . |
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Catalytic combustion holds great promise for eliminating unburned methane released by the natural gas industry, and the crucial factor is the development of cost-effective and efficient catalysts. Herein, the silicon component was introduced into nickel oxide by simultaneously regulating the precipitation of nickel precursors and the hydrolysis of silicon precursors. The generation of SiO4 groups in NiO inhibited the growth and sintering of NiO grains, meanwhile promoting the formation of active Ni2+ and adsorbed oxygen species for activation and oxidation of methane. With the increase of Si content, the existence of surface nickel silicate on NiO further improved the sinter resistance of NiO, but caused the diminish of Ni2+ and surface adsorbed oxygen species. The catalytic activity and stability were co-enhanced via facilely tuning the multiple Ni-Si interactions. The catalyst with abundant SiO4 groups and negligible nickel silicate exhibited considerably higher catalytic activity, sinter-resistance and water-resistance than NiO toward methane combustion.
Keyword ：
Catalytic activity Catalytic activity Methane combustion Methane combustion Multiple Ni-Si interaction Multiple Ni-Si interaction NiO-based catalysts NiO-based catalysts Thermal stability Thermal stability
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| GB/T 7714 | Wang, Zhixiong , Tang, Chenyao , Lin, Jia et al. Promoting methane combustion activity and stability by tuning multiple Ni-Si interactions in catalysts [J]. | FUEL , 2023 , 349 . |
| MLA | Wang, Zhixiong et al. "Promoting methane combustion activity and stability by tuning multiple Ni-Si interactions in catalysts" . | FUEL 349 (2023) . |
| APA | Wang, Zhixiong , Tang, Chenyao , Lin, Jia , Zheng, Yong , Xiao, Yihong , Zheng, Ying et al. Promoting methane combustion activity and stability by tuning multiple Ni-Si interactions in catalysts . | FUEL , 2023 , 349 . |
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天然气、油田伴生气、高炉煤气等化工生产过程中伴生COS气体，不仅会腐蚀管道和毒害催化剂，还会严重污染环境并危害人类健康。COS催化水解反应可在温和条件下高效的将COS脱除，是最具应用前景的COS脱除技术之一。碱金属元素因其具有独特的电子供体性质、表面碱性和静电吸附等特性，常被用作助催化剂以提高Al_2O_3的COS催化水解性能。近年来，以钾为助剂改性的Al_2O_3催化剂(K_2CO_3/Al_2O_3)在COS催化水解反应中得到广泛的应用，但由于负载在Al_2O_3上的K物种的组成复杂，目前研究者对K_2CO_3/Al_2O_3催化剂上COS水解机理的理解仍存在一定的困惑和争议。本论文通过湿法浸渍法合成出一系列钾盐和钠盐改性的Al_2O_3催化剂，并利用各类先进的表征技术对这些催化剂进行分析。活性测试表明，以K_2CO_3、K_2C_2O_4、NaHCO_3、Na_2CO_3和NaC_2O_4改性Al_2O_3催化剂均有助于COS的水解。其中K_2CO_3/Al_2O_3拥有最佳的COS水解性能，连续运行20 h后其COS转化率仍高于～93%，远远优于未改性的Al_2O_3 (～58%)。我们利用原位红外光谱和X射线光电子能谱探明了反应过程中催化剂的化学结构特征，阐明了H_2O分子在K_2CO_3/Al_2O_3上的水解作用机制。原位红外表明COS在K_2CO_3/Al_2O_3上的水解过程中形成了硫代碳酸氢盐中间产物。X射线光电子能谱表征证明催化剂的失活主要是因为催化剂表面积累了硫酸盐和单质硫。此外，我们还研究了水蒸气含量对COS水解性能的影响，研究发现，由于H_2O和COS分子在催化剂表面存在竞争吸附，过量的H_2O会引起催化活性的下降。上述研究表明，K_2CO_3/Al_2O_3催化剂上COS水解性能的提高主要是形成了HO-Al-O-K界面活性位。更为重要的是，所制备的催化剂都是在模拟工业工况条件下进行的，这为后续的工业应用提供了宝贵理论指导。本工作为理解助剂钾在Al_2O_3催化剂上COS水解活性的增强提供了新的见解，这为未来设计稳定高效的COS水解催化剂打开了新的发展方向。
Keyword ：
HO-Al-O-K界面活性位点 HO-Al-O-K界面活性位点 催化水解 催化水解 失活机理 失活机理 工业工况条件 工业工况条件 羰基硫 羰基硫
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| GB/T 7714 | 雷淦昌 , 郑勇 , 曹彦宁 et al. 钾改性氧化铝基羰基硫水解催化剂及其失活机理（英文） [J]. | 物理化学学报 , 2023 , 39 (09) : 115-124 . |
| MLA | 雷淦昌 et al. "钾改性氧化铝基羰基硫水解催化剂及其失活机理（英文）" . | 物理化学学报 39 . 09 (2023) : 115-124 . |
| APA | 雷淦昌 , 郑勇 , 曹彦宁 , 沈丽娟 , 王世萍 , 梁诗景 et al. 钾改性氧化铝基羰基硫水解催化剂及其失活机理（英文） . | 物理化学学报 , 2023 , 39 (09) , 115-124 . |
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The development of efficient and stable nanocatalysts is crucial for the catalytic removal of H2S through selective oxidation to sulfur. Inspired by the different catalytic activity and selectivity of CeO2 and MnO2 for the reaction, cerium-manganese (Ce-Mn) nanocomposite oxides with tunable phase structure and unique surface properties were constructed to optimize the catalytic performance. By regulating the molar ratio of Ce and Mn components, a novel catalyst structure comprising Ce-Mn solid solution and amorphous CeO2 is synthesized from Ce-Mn oxide with n(Ce)/n(Mn) ratio of 0.5 (50Ce-Mn). Compared with the unmodified MnO2, the tailored 50Ce-Mn possesses a high specific surface area, which facilitates the access of reactants to active sites and the desorption of formed sulfur. More importantly, strong Ce-Mn interaction and abundant surface-active oxygen species are generated, contributing to the regeneration of Mn4+/Ce4+ active sites, facilitating the formation of sulfur, and inhibiting the accumulation of sulfates during the reaction. Consequently, 50Ce-Mn presents a superior catalytic activity (T-100 of 150 degrees C), stability, and sulfur selectivity even under relatively high weight hourly space velocity conditions (23,000 mL center dot g(-1)center dot h(-1)). This study provides an example of how catalytic performance can be boosted through phase structure regulation on nanocomposites.
Keyword ：
cerium-manganese nanocatalysts cerium-manganese nanocatalysts electron transfer electron transfer H2S-selective catalytic oxidation H2S-selective catalytic oxidation oxygen vacancy oxygen vacancy phase structure phase structure
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| GB/T 7714 | Zhang, Qiongdan , Zheng, Chengcheng , Zhang, Ke et al. Ce-Mn Oxide Nanocomposites for Catalytic Removal of H2S [J]. | ACS APPLIED NANO MATERIALS , 2023 , 6 (4) : 2585-2595 . |
| MLA | Zhang, Qiongdan et al. "Ce-Mn Oxide Nanocomposites for Catalytic Removal of H2S" . | ACS APPLIED NANO MATERIALS 6 . 4 (2023) : 2585-2595 . |
| APA | Zhang, Qiongdan , Zheng, Chengcheng , Zhang, Ke , Zheng, Yong , Xiao, Yihong , Jiang, Lilong . Ce-Mn Oxide Nanocomposites for Catalytic Removal of H2S . | ACS APPLIED NANO MATERIALS , 2023 , 6 (4) , 2585-2595 . |
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