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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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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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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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针对传统两级式LED驱动电源中存在着半导体功率器件数目多,控制电路复杂,效率低,成本高,可靠性差等问题,提出一种单级无桥Sepic谐振LED驱动电路,通过将单开关无桥Sepic电路主开关管与半桥LLC电路下开关管复用集成单级LED驱动电路,减少了半导体功率器件数目,简化控制电路,提高了电路效率和工作可靠性.详细分析了所提出电路的工作原理和工作过程,深入开展了电路输入输出电压变比、网侧特性、软开关特性等稳态特性推导和电路关键参数设计,并针对所提出单级电路由于输入电压变化引起直流母线电压变动范围大等问题,分析设计了一种APWM-PFM混合控制策略.最后进行计算机仿真分析,并设计一台交流输入185～265 Vrms、额定输出2A/96W的实验样机,样机效率最高可达91.5%,PF最大值为0.995,THD最小为5.5%,不同交流电压下直流母线电压总体变化范围在60V以内,实现直流母线电压限压.计算机仿真结果和实验结果验证所提出电路和混合控制策略的理论预期和有效性.
Keyword ：
LED照明 LED照明 功率因数校正 功率因数校正 单级无桥Sepic/LLC电路 单级无桥Sepic/LLC电路 直流母线电压APWM-PFM混合控制 直流母线电压APWM-PFM混合控制 软开关 软开关
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| GB/T 7714 | 林中寅 , 林维明 , 黄舒晨 et al. 单级无桥Sepic谐振LED驱动电路及其APWM-PFM混合控制 [J]. | 电机与控制学报 , 2024 , 28 (9) : 106-124 . |
| MLA | 林中寅 et al. "单级无桥Sepic谐振LED驱动电路及其APWM-PFM混合控制" . | 电机与控制学报 28 . 9 (2024) : 106-124 . |
| APA | 林中寅 , 林维明 , 黄舒晨 , 郑勇 . 单级无桥Sepic谐振LED驱动电路及其APWM-PFM混合控制 . | 电机与控制学报 , 2024 , 28 (9) , 106-124 . |
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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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Carbonyl sulfide (COS) is commonly found in conventional fossil fuels, such as nature gas, oil-associated gas, and blast-furnace gas, and its untreated emission not only corrodes pipelines and poisons catalysts but will also inevitably pollute the environment and endanger human health. Catalytic hydrolysis is recognized as the most promising strategy to eliminate COS because it can be performed under mild reaction conditions with a high removal efficiency. Notably, alkali metals promote catalytic COS hydrolysis over Al2O3 owing to their electron donor properties, basicity, and electrostatic adsorption. However, despite the significant attraction of using potassium-promoted Al2O3 (K2CO3/Al2O3) as conventional catalysts for COS hydrolysis, the mechanism of COS hydrolysis over K2CO3/Al2O3 remains unclear and is controversial owing to the complex composition of the K species. In this study, commercial Al2O3 modified with potassium and sodium salts were synthesized using the wet impregnation method and characterized by various techniques. Based on the results of the activity measurements, the K2CO3-, K2C2O4-, NaHCO3-, Na2CO3-, and NaC2O4-modified catalysts had a positive effect on COS hydrolysis. Among them, the K2CO3/Al2O3 catalyst exhibited the highest COS conversion. Notably, the K2CO3/Al2O3 catalyst exhibited an excellent catalytic performance (-93%, 20 h), which is significantly better than that of pristine Al2O3 (-58%). Furthermore, this study provides strong evidence for the role of H2O during catalytic hydrolysis over K2CO3/Al2O3 using in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and X-ray photoelectron spectroscopy (XPS). The in situ DRIFTS analysis revealed that hydrogen thiocarbonate formed as an intermediate during COS hydrolysis over K2CO3/Al2O3. Meanwhile, the XPS findings suggested that sulfates and elemental sulfur accumulated on the catalyst surface, which may have contributed to catalyst poisoning. Additionally, the effect of water vapor content in the reaction pathway of COS hydrolysis over K2CO3/Al2O3 was investigated. The presence of excess water resulted in a reduction in catalytic activity owing to competitive adsorption between H2O and COS molecules on the catalyst surface. The enhancement in the catalytic activity over K2CO3/Al2O3 may be attributed to the formation of HO-Al-O-K interfacial sites. More importantly, all the catalysts were used under industrially relevant conditions, which provides valuable theoretical guidance for practical applications in the future. Thus, this detailed mechanistic study reveals new insights into the roles of the interfacial K co -catalyst, which provides a new opportunity for the rational design of stable and efficient catalysts for COS hydrolysis.
Keyword ：
Carbonyl sulfide Carbonyl sulfide Catalytic hydrolysis Catalytic hydrolysis Deactivation mechanism Deactivation mechanism HO-Al-O-K interface site HO-Al-O-K interface site Industrial-relevant condition Industrial-relevant condition
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| GB/T 7714 | Lei, Ganchang , Zheng, Yong , Cao, Yanning et al. Deactivation Mechanism of COS Hydrolysis over Potassium Modified Alumina [J]. | ACTA PHYSICO-CHIMICA SINICA , 2023 , 39 (9) . |
| MLA | Lei, Ganchang et al. "Deactivation Mechanism of COS Hydrolysis over Potassium Modified Alumina" . | ACTA PHYSICO-CHIMICA SINICA 39 . 9 (2023) . |
| APA | Lei, Ganchang , Zheng, Yong , Cao, Yanning , Shen, Lijuan , Wang, Shiping , Liang, Shijing et al. Deactivation Mechanism of COS Hydrolysis over Potassium Modified Alumina . | ACTA PHYSICO-CHIMICA SINICA , 2023 , 39 (9) . |
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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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The activation of H2O is a key step of the COS hydrolysis,which may be tuned by oxygen vacancy defects in the catalysts.Herein,we have introduced Cu into Co3O4 to regulate the oxygen vacancy defect content of the catalysts.In situ DRIFTS and XPS spectra reveal that COS and H2O are adsorbed and activated by oxygen vacancy.The 10 at％Cu doped Co3O4 sample(10Cu-Co3O4)exhibits the optimal activity,100％of COS conversion at 70 ℃.The improved oxygen vacancies of Cu-Co3O4 accelerate the activation of H2O to form active-OH.COS binds with hydroxyl to form the intermediate HSCO2,and then the activated-OH on the oxygen vacancy reacts with HSCO2 to form HCO3.Meanwhile,the catalyst exhibits high catalytic stability because copper species(Cu+/Cu2+)redox cycle mitigate the sulfation of Co3O4(Co2+/Co3+).Our work offers a promising approach for the rational design of cobalt-related catalysts in the highly efficient hydrolysis COS process.
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| GB/T 7714 | Guanyu Mu , Yan Zeng , Yong Zheng et al. Oxygen vacancy defects engineering on Cu-doped Co3O4 for promoting effective COS hydrolysis [J]. | 绿色能源与环境（英文版） , 2023 , 8 (3) : 831-841 . |
| MLA | Guanyu Mu et al. "Oxygen vacancy defects engineering on Cu-doped Co3O4 for promoting effective COS hydrolysis" . | 绿色能源与环境（英文版） 8 . 3 (2023) : 831-841 . |
| APA | Guanyu Mu , Yan Zeng , Yong Zheng , Yanning Cao , Fujian Liu , Shijing Liang et al. Oxygen vacancy defects engineering on Cu-doped Co3O4 for promoting effective COS hydrolysis . | 绿色能源与环境（英文版） , 2023 , 8 (3) , 831-841 . |
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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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