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学者姓名：肖益鸿
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Abstract ：
Catalytic combustion shows promise in mitigating methane emissions from natural gas utilization, while the presence of sulfur species in natural gas can cause significant catalyst deactivation. Herein, a dual-modification strategy is proposed to construct active and sulfur-resistant nickel oxide (NiO)-based catalysts. Through regulating the hydrolysis of the silicon (Si) precursor and the precipitation of zirconium (Zr) and nickel (Ni) precursors, both the Si and Zr component could enter NiO lattice to generate strong interactions, leading to a decrease in crystallite size, an increase in active Ni2+ and surface adsorbed oxygen species for the efficient methane combustion. The incorporation of Si prominently enhanced the surface acidity of catalysts to inhibit the sulfating of NiO; the introduced Zr component also contributed to the generation of surface acid sites, and had a preferential interaction with sulfur dioxide (SO2) to protect Ni2+ sites. Consequently, the small NiO crystallites, active Ni2+ and oxygen species could be maintained in dual-modified catalysts under sulfur-containing reaction conditions, leading to the superior catalytic performance compared to NiO or catalysts modified by Zr or Si. This work introduces a practical and efficient approach for developing catalysts to remove gaseous pollutants.
Keyword ：
Catalytic combustion of methane Catalytic combustion of methane Modified NiO Modified NiO Si and Zr-incorporation Si and Zr-incorporation Sulfur-resistance Sulfur-resistance Surface acidity Surface acidity
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| GB/T 7714 | Tian, Chengchen , Lin, Jia , Lin, Li et al. A silicon-zirconium dual-modified nickel oxide with high activity and sulfur-resistance for catalytic combustion removal of methane [J]. | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING , 2024 , 13 (1) . |
| MLA | Tian, Chengchen et al. "A silicon-zirconium dual-modified nickel oxide with high activity and sulfur-resistance for catalytic combustion removal of methane" . | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING 13 . 1 (2024) . |
| APA | Tian, Chengchen , Lin, Jia , Lin, Li , Zheng, Yong , Xiao, Yihong , Zheng, Ying . A silicon-zirconium dual-modified nickel oxide with high activity and sulfur-resistance for catalytic combustion removal of methane . | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING , 2024 , 13 (1) . |
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It is essential to develop catalysts that demonstrate outstanding catalytic activity and N2 selectivity to effectively purify NH3-containing waste gas through selective oxidation of NH3. Herein, we present a facile strategy to construct high-performance CuO-based catalysts through the incorporation of niobium (Nb) component. The Nb species with molar ratios of 0.05-0.2 could enter the CuO lattice and generate Cu-O-Nb bonds, resulting in lattice distortion and weakened Cu-O bond, which enhanced the redox properties as well as surface acidity of CuO. The catalytic activity was improved by the increased Cu+, surface chemisorbed oxygen species, and weak acid sites, while N2 selectivity was promoted mainly due to the generation of moderate and strong acid sites. The catalyst with a relatively low content of Nb (molar ratio of 0.1) exhibited optimal redox properties and surface acidity, which facilitated the reaction to proceed through both imide and i-SCR mechanisms, resulting in significantly enhanced catalytic activity, stability, and N2 selectivity compared to CuO. This investigation underscores the importance of dual modification of redox properties and surface acidity of catalysts for improving catalytic performance.
Keyword ：
CuO-based catalysts CuO-based catalysts Nb-incorporation Nb-incorporation NH 3-SCO reaction NH 3-SCO reaction Redox property Redox property Surface acidity Surface acidity
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| GB/T 7714 | Pang, Lei , Gao, Mengjie , Lin, Jia et al. Redox-acidity dual modification of CuO by niobium-incorporation for enhanced selective catalytic oxidation of NH3 [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 354 . |
| MLA | Pang, Lei et al. "Redox-acidity dual modification of CuO by niobium-incorporation for enhanced selective catalytic oxidation of NH3" . | SEPARATION AND PURIFICATION TECHNOLOGY 354 (2024) . |
| APA | Pang, Lei , Gao, Mengjie , Lin, Jia , Zheng, Yong , Xiao, Yihong , Zheng, Ying et al. Redox-acidity dual modification of CuO by niobium-incorporation for enhanced selective catalytic oxidation of NH3 . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 354 . |
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The efficient adsorption of sulfur dioxide (SO2) is crucial for purifying exhaust gases, and zeolites are promising adsorbents due to their low cost and excellent stability. However, developing FAU-type zeolites with high adsorption capacities and selectivities remains challenging due to their narrow pores and limited adsorption sites. Herein, an additive-free synthesis strategy is proposed to facilely obtain NaX zeolites (X-HCL) with the house-of-card-like morphology. The hierarchical structure of X-HCL not only benefits the removal of SO2 through favorable spatial diffusion, but also promotes the loading of basic adsorption sites- [caprolactam] [tetrabutylammonium bromide] (CT) ionic liquid. The obtained CT/X-HCL adsorbent demonstrates remarkable SO2 adsorption capacity (10.58 mmol/g) and cyclic stability, as well as great selectivity of SO2/N-2 (1673) and SO2/ CO2 (219) due to the strong affinity of CT towards SO2. Moreover, co-feeding with water vapor benefits the adsorption of SO2 on CT/X-HCL owing to the enhanced chemisorption of hydrated CT for SO2. This research provides new insights into the construction of hierarchical zeolite for efficient adsorption and separation of SO2.
Keyword ：
Hierarchical Hierarchical House-of-card-like morphology House-of-card-like morphology Ionic liquid Ionic liquid NaX zeolite NaX zeolite Sulfur dioxide adsorption Sulfur dioxide adsorption
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| GB/T 7714 | Zhang, Qiongdan , Ye, Ming , Lei, Yuanyi et al. Additive-free synthesis of house-of-card NaX zeolite for supporting amine: An efficient adsorbent for SO2 removal [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 354 . |
| MLA | Zhang, Qiongdan et al. "Additive-free synthesis of house-of-card NaX zeolite for supporting amine: An efficient adsorbent for SO2 removal" . | SEPARATION AND PURIFICATION TECHNOLOGY 354 (2024) . |
| APA | Zhang, Qiongdan , Ye, Ming , Lei, Yuanyi , Wang, Heng , Zheng, Yong , Xiao, Yihong et al. Additive-free synthesis of house-of-card NaX zeolite for supporting amine: An efficient adsorbent for SO2 removal . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 354 . |
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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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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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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 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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In this work, metal oxides with different phase structures (stannic oxide, zirconia and tin-zirconium binary oxide) were designed to construct palladium-based catalysts. The factors affecting methane combustion over catalysts were revealed by exploring the reasons for the enhancement and depression of catalytic performance under various reaction conditions. The formation of SnxZr1_ xO2 solid solutions not only generated abundant oxygen vacancies to improve the reducibility of PdO and the redox of Pd <-> PdO, but also induced the formation of active PdOx, conjointly leading to the excellent catalytic activity and hydrothermal stability. Under SO2-containing atmosphere, the thermodynamically favorable formation of stable Zr(SO4)2 caused the significant diminish of oxygen vacancies and active Pd step sites in catalysts. Consequently, the sulfur-resistance and regeneration performance of Zr-containing catalysts were inferior to those of Pd/SnO2. The above contrast manifested that both oxygen vacancies and active palladium species were responsible for the efficient and stable methane combustion.
Keyword ：
Methane combustion Methane combustion Oxygen vacancies Oxygen vacancies Palladium catalysts Palladium catalysts Sn x Zr 1_x O 2 solid solutions Sn x Zr 1_x O 2 solid solutions Support effect Support effect
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| GB/T 7714 | Lin, Jia , Huang, Jiangli , Chen, Xiaohua et al. Key factors for methane combustion over palladium-based catalysts revealed by enhanced and depressed catalytic performance [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2023 , 340 . |
| MLA | Lin, Jia et al. "Key factors for methane combustion over palladium-based catalysts revealed by enhanced and depressed catalytic performance" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 340 (2023) . |
| APA | Lin, Jia , Huang, Jiangli , Chen, Xiaohua , Zheng, Yong , Xiao, Yihong , Zheng, Ying et al. Key factors for methane combustion over palladium-based catalysts revealed by enhanced and depressed catalytic performance . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2023 , 340 . |
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本发明涉及一种用于有机硫催化水解的复合金属氧化物的制备方法，其利用无溶剂合成方法，通过搅拌来达到金属间的均匀分散，再通过高温煅烧获得氧化铈掺杂镍。在煅烧的过程中，前驱体中的气体在高温情况下发生分解并以气体的形式排到环境中，促进催化剂形成孔道结构。该方法合成条件简单且反应迅速，耗时短，在制备过程中无需加入任何的溶剂，原子利用率高且无任何废水产生。在温度为90℃下便具有高达100%COS转化率，适用于中低温催化水解羰基硫气体。
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| GB/T 7714 | 江莉龙 , 朱棋良 , 刘福建 et al. 一种用于有机硫催化水解的复合金属氧化物的制备方法 : CN202210154143.2[P]. | 2022-02-21 00:00:00 . |
| MLA | 江莉龙 et al. "一种用于有机硫催化水解的复合金属氧化物的制备方法" : CN202210154143.2. | 2022-02-21 00:00:00 . |
| APA | 江莉龙 , 朱棋良 , 刘福建 , 梁诗景 , 郑勇 , 曹彦宁 et al. 一种用于有机硫催化水解的复合金属氧化物的制备方法 : CN202210154143.2. | 2022-02-21 00:00:00 . |
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We report herein a facile pyrolysis etching strategy for the fabrication of UiO-66-xs single crystals with tunable coordination unsaturated zirconium sites (Zr-CUS) as well as interconnected mesoporosity. The synthesis is realized by having pristine UiO-66-xs subjected to thermal treatment, which results in the selective decompo-sition of thermal-sensitive organic linkers and hence the creation of permanent mesoporosity, leaving abundant Zr-CUS with enhanced degree of exposure. The prepared hierarchically porous UiO-66-xs (HP-UiO-66-xs) were innovatively applied for mild oxidation of H2S into polysulphur, achieving near 100 % H2S conversion and polysulphur selectivity in a wide range of temperatures. The superior activities can be well maintained in a continuous test of over 50 h. The Zr-CUS of HP-UiO-66-xs effectively activate H2S and O2 via the "adsorption dissociation tandem hydrogen transfer" mechanism, and the abundant mesochannels ensure efficient transport of reactants and bulky products in and out HP-UiO-66-xs, leading to catalytic activities superior to those of traditional H2S selective oxidation catalysts.
Keyword ：
Coordination unsaturated degree Coordination unsaturated degree H2S selective oxidation H2S selective oxidation Mass transportation Mass transportation Mesoporous metal organic frameworks Mesoporous metal organic frameworks Polysulphur catalytic synthesis Polysulphur catalytic synthesis
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| GB/T 7714 | Zhang, Guanqing , Liu, Fengqing , Qu, Yongfang et al. Controllable creating mesoporous coordination unsaturated sites in UiO-66 single crystals for efficient conversion of hydrogen sulfide into polysulphur [J]. | CHEMICAL ENGINEERING JOURNAL , 2023 , 479 . |
| MLA | Zhang, Guanqing et al. "Controllable creating mesoporous coordination unsaturated sites in UiO-66 single crystals for efficient conversion of hydrogen sulfide into polysulphur" . | CHEMICAL ENGINEERING JOURNAL 479 (2023) . |
| APA | Zhang, Guanqing , Liu, Fengqing , Qu, Yongfang , Zheng, Yong , Cao, Yanning , Liu, Fujian et al. Controllable creating mesoporous coordination unsaturated sites in UiO-66 single crystals for efficient conversion of hydrogen sulfide into polysulphur . | CHEMICAL ENGINEERING JOURNAL , 2023 , 479 . |
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