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Cu/Co/Fe浸渍ZSM-催/MOR型分子筛选择性化燃烧5/乙BE腈A乙烷性能
期刊论文 | 2023 , 41 (S2) , 460-467 | 环境工程
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Abstract :

含氰废气作为一类挥发性有机物,具有剧毒性和致癌性,较低浓度的排放即可对人类健康造成严重危害,其在金属改性沸石催化剂上的选择性催化燃烧因其高效性和产物高选择性备受关注。以乙腈、乙烷作为含氰废气的典型组分,采用浸渍法制备了(2%、3%、5%、7%、10%)Cu、Fe、Co/ZSM-5、BEA、MOR催化剂,考察了其含氰废气选择性催化燃烧活性。选择性能优异的催化剂,运用XRD、氮气吸附-脱附、NH_3-TPD、H_2-TPR、XPS和EPR等手段对催化剂的理化性质进行了表征。7%Cu-ZSM-5的催化活性最佳,300℃实现了乙腈和乙烷的完全转化,N_2产率最高达97%。结果表明催化剂的氧化还原能力是决定含氰废气催化燃烧效率的决定性因素,金属的化学性质对含氰废气的转化率具有重要影响作用,N_2的选择性是由催化剂的酸性强弱、氧化还原能力以及分子筛的拓扑结构共同决定的。

Keyword :

选择催化燃烧 选择催化燃烧 含氰废气 含氰废气 分子筛 分子筛 表面改性 表面改性

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GB/T 7714 郭重阳 , 刘宁 , 陈标华 . Cu/Co/Fe浸渍ZSM-催/MOR型分子筛选择性化燃烧5/乙BE腈A乙烷性能 [J]. | 环境工程 , 2023 , 41 (S2) : 460-467 .
MLA 郭重阳 等. "Cu/Co/Fe浸渍ZSM-催/MOR型分子筛选择性化燃烧5/乙BE腈A乙烷性能" . | 环境工程 41 . S2 (2023) : 460-467 .
APA 郭重阳 , 刘宁 , 陈标华 . Cu/Co/Fe浸渍ZSM-催/MOR型分子筛选择性化燃烧5/乙BE腈A乙烷性能 . | 环境工程 , 2023 , 41 (S2) , 460-467 .
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超临界CO_2在废旧聚酯纺织品脱色中的性能研究
期刊论文 | 2023 , 41 (S2) , 622-627 | 环境工程
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聚对苯二甲酸乙二醇酯(PET)纺织品因其优异的性能受到青睐,已成为纺织面料的中流砥柱。为满足人类生产生活的需要,彩色聚酯纺织品的消费量是巨大的。废旧聚酯产品难以降解,对环境污染严重,但由于PET纺织品中含有染料等添加剂,使得PET纺织品再生利用率低。本研究将超临界CO_2引入原液着色聚酯脱色工作中,分别考察了N,N-二甲基甲酰胺(DMF)和二甲基亚砜(DMSO)在超临界CO_2下对原液着色PET织物的脱色性能。此外,还将超临界CO_2脱色与常规方式脱色进行比较。结果表明:DMF和DMSO在超临界CO_2条件下能充分发挥其脱色性能,并且DMF对聚酯的脱色效果优于DMSO。在脱色剂(DMF)、液比(1∶15)、处理时间(20 min)、温度(140℃)和压力(10 MPa)的优化组合下,PET织物具有良好的脱色效果。通过NMR、GPC、TG、DSC、XRD和醇解实验考察了超临界CO_2脱色后PET织物的性能。

Keyword :

脱色 脱色 聚酯 聚酯 聚酯回收 聚酯回收 超临界二氧化碳 超临界二氧化碳 聚酯纺织品 聚酯纺织品

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GB/T 7714 王星丽 , 于刚强 , 吴宝宅 et al. 超临界CO_2在废旧聚酯纺织品脱色中的性能研究 [J]. | 环境工程 , 2023 , 41 (S2) : 622-627 .
MLA 王星丽 et al. "超临界CO_2在废旧聚酯纺织品脱色中的性能研究" . | 环境工程 41 . S2 (2023) : 622-627 .
APA 王星丽 , 于刚强 , 吴宝宅 , 王钱 , 刘宁 , 代成娜 et al. 超临界CO_2在废旧聚酯纺织品脱色中的性能研究 . | 环境工程 , 2023 , 41 (S2) , 622-627 .
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Mechanistic Insight into the Propane Oxidation Dehydrogenation by N2O over Cu-BEA Zeolite with Diverse Active Site Structures SCIE
期刊论文 | 2023 , 13 (8) | CATALYSTS
WoS CC Cited Count: 2
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Abstract :

The present work theoretically investigated propane oxidation dehydrogenation by utilizing N2O as an oxidant (N2O-ODHP) over Cu-BEA with three different types of active site, including monomeric Cu ([Cu](+)), dimeric Cu ([Cu-Cu](2+)), and distant monomeric Cu sites ([Cu](+)-[Cu](+)). Energetically, we calculated that the monomeric [Cu]+ is favorable for the aH dehydrogenation step (6E = 0.05 eV), which, however, suffers from high barriers of N2O dissociation and (3H dehydrogenation steps of 1.40 and 1.94 eV, respectively. Although the dimeric [Cu-Cu](2+) site with a Cu-Cu distance of 4.91 & Aring; is much more favorable for N2O dissociation (0.95 eV), it still needs to overcome an extremely high barrier (6E = 2.15 eV) for (3H dehydrogenation. Interestingly, the distant [Cu](+)-[Cu](+) site with the Cu-Cu distance of 5.82 & Aring; exhibits low energy barriers for N2O dissociation (0.89 eV) and ODHP steps (0.01 and 0.33 eV) due to the synergistic effect of distant [Cu](+). The microkinetic analyses quantitatively verified the superior activity of the distant [Cu](+)-[Cu](+) site with a reaction rate being eight to nine orders of magnitude higher than those of the monomeric and the dimeric Cu sites, and this is related to its ready charge-transfer ability, as shown by the partial Density of State (PDOS) analysis and the static charge differential density analysis in this study. Generally, the present work proposes that the distance between the [Cu](+) sites plays a significant and important role in N2O-ODHP over the Cu-based zeolite catalyst and modulates Cu-Cu distance, and this constitutes a promising strategy for highly-efficient Cu-zeolite catalyst design for N2O-ODHP.

Keyword :

Cu-BEA Cu-BEA N2O N2O propane oxidation dehydrogenation (ODHP) propane oxidation dehydrogenation (ODHP) density functional theory (DFT) density functional theory (DFT) microkinetic modelling microkinetic modelling

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GB/T 7714 Wu, Ruiqi , Liu, Ning , Dai, Chengna et al. Mechanistic Insight into the Propane Oxidation Dehydrogenation by N2O over Cu-BEA Zeolite with Diverse Active Site Structures [J]. | CATALYSTS , 2023 , 13 (8) .
MLA Wu, Ruiqi et al. "Mechanistic Insight into the Propane Oxidation Dehydrogenation by N2O over Cu-BEA Zeolite with Diverse Active Site Structures" . | CATALYSTS 13 . 8 (2023) .
APA Wu, Ruiqi , Liu, Ning , Dai, Chengna , Xu, Ruinian , Yu, Gangqiang , Wang, Ning et al. Mechanistic Insight into the Propane Oxidation Dehydrogenation by N2O over Cu-BEA Zeolite with Diverse Active Site Structures . | CATALYSTS , 2023 , 13 (8) .
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Mesoscale study of crystal-plane effects of Ni catalysts on CO2 hydrogenation SCIE
期刊论文 | 2023 , 25 (23) , 16105-16113 | PHYSICAL CHEMISTRY CHEMICAL PHYSICS
WoS CC Cited Count: 2
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Crystal-plane effects have pivotal roles in the design of catalysts. In this study, a branched Ni (Ni-BN) catalyst was mainly exposed at the Ni(322) surface and was synthesized in the presence of H-2. A Ni nanoparticle (Ni-NP) catalyst was mainly exposed at Ni(111) and Ni(100) surfaces and was synthesized without H-2. The Ni-BN catalyst showed higher CO2 conversion and methane selectivity than the Ni-NP catalyst. DRIFTS revealed that, unlike the formate route for methanation over the Ni-BN catalyst, the main methanation pathway over the Ni-NP catalyst was the CO2 direct dissociation route, which revealed that the diversity of reaction mechanisms of CO2 methanation on different crystal planes led to the disparity in catalyst activity. DFT calculation of the CO2 hydrogenation reaction over various surfaces showed that the energy barriers on Ni(110) and Ni(322) surfaces were lower than those of Ni(111) and Ni(100) surfaces, which was also related to different pathways of the reaction mechanism. Microkinetic analysis showed the reaction rates on Ni(110) and Ni(322) surfaces were higher than those of other surfaces, and CH4 was the main product on all calculated surfaces, whereas the yields of CO on Ni(111) and Ni(100) surfaces were higher. Kinetic Monte Carlo simulations revealed that the Ni(322) surface with stepped sites was responsible for CH4 generation, and that simulated methane selectivity was consistent with experimental results. The crystal-plane effects of the two morphologies of Ni nanocrystals explained why the reaction activity of the Ni-BN catalyst was greater than that of the Ni-NP catalyst.

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GB/T 7714 Wang, Xiaolei , Liu, Ning , Xu, Ruinian et al. Mesoscale study of crystal-plane effects of Ni catalysts on CO2 hydrogenation [J]. | PHYSICAL CHEMISTRY CHEMICAL PHYSICS , 2023 , 25 (23) : 16105-16113 .
MLA Wang, Xiaolei et al. "Mesoscale study of crystal-plane effects of Ni catalysts on CO2 hydrogenation" . | PHYSICAL CHEMISTRY CHEMICAL PHYSICS 25 . 23 (2023) : 16105-16113 .
APA Wang, Xiaolei , Liu, Ning , Xu, Ruinian , Chen, Biaohua , Dai, Chengna , Yu, Gangqiang . Mesoscale study of crystal-plane effects of Ni catalysts on CO2 hydrogenation . | PHYSICAL CHEMISTRY CHEMICAL PHYSICS , 2023 , 25 (23) , 16105-16113 .
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一种使用疏水性低共熔溶剂从废电池中选择性分离锂与过渡金属的协同萃取方法 incoPat
专利 | 2022-06-29 | CN202210750305.9
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一种使用疏水性低共熔溶剂从废电池中选择性分离锂与过渡金属的协同萃取方法属湿法冶金技术领域,提供一种分离与提取效果好的协同萃取方法,具体公开了一种疏水性低共熔与磷酸三丁酯(TBP)协同萃取剂及分离废锂电池浸出液中的锂与过渡金属的方法,本申请提供的疏水性低共熔包含正癸酸(氢键供体)与利多卡因(氢键受体)。所述方法包括如下步骤:(1)配置疏水性低共熔溶剂;(2)配置萃取有机相;(3)镍钴锰共萃;(4)镍钴锰反萃;(5)锂沉淀。本发明对镍钴锰过渡金属的萃取效果好,剩余水相中锂的纯度高,实现对废锂电池正极材料浸出液中有价金属的高效回收,且使用的低共熔溶剂污染小、合成简便、价格低,是一种“新型绿色”溶剂。

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GB/T 7714 陈标华 , 郭宇 , 于刚强 et al. 一种使用疏水性低共熔溶剂从废电池中选择性分离锂与过渡金属的协同萃取方法 : CN202210750305.9[P]. | 2022-06-29 .
MLA 陈标华 et al. "一种使用疏水性低共熔溶剂从废电池中选择性分离锂与过渡金属的协同萃取方法" : CN202210750305.9. | 2022-06-29 .
APA 陈标华 , 郭宇 , 于刚强 , 代成娜 , 刘宁 , 徐瑞年 et al. 一种使用疏水性低共熔溶剂从废电池中选择性分离锂与过渡金属的协同萃取方法 : CN202210750305.9. | 2022-06-29 .
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H2O in situ induced active site structure dynamics for efficient methane direct oxidation to methanol over Fe-BEA zeolite br SCIE
期刊论文 | 2022 , 414 , 302-312 | JOURNAL OF CATALYSIS
WoS CC Cited Count: 9
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The H2O has recently aroused great attentions due to its special promotion effect during direct oxidation of methane to methanol (DMTM). Herein, the H2O is for the first time unravelled working as one type of active site tuning agent that can in situ transform the active site from less active [Fe-O-Fe]2+ into highly active [FeOH]2+-O-[FeOH]2+ (assisted by N2O) over the best performing Fe-BEA-1 % during continuous N2O-DMTM (T = 250 degrees C). Specifically, the generated radicals of CH3- and OH-prefer to react with the [OH]-groups of [FeOH]2+-O-[FeOH]2+ to respectively produce CH3OH and regenerate H2O following a favorable energy route (<0.6 eV), eventually leading to pronouncedly boosted CH3OH productivity (from 25.0 to 227.0 lmol g-1h-1), selectivity (from 9.4 to 72.9 %) and long-term reaction stability. The present work sheds a new light on the active site structure directing effect of H2O, which would substantially favor other highly efficient catalyst designs. (c) 2022 Elsevier Inc. All rights reserved.

Keyword :

(DMTM) (DMTM) Fe-BEA Fe-BEA H2O induced active site structure dynamics H2O induced active site structure dynamics [Fe(OH)]2+-O-[Fe(OH)]2+ [Fe(OH)]2+-O-[Fe(OH)]2+ N2O N2O Direction oxidation of methane to methanol&nbsp Direction oxidation of methane to methanol&nbsp

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GB/T 7714 Liu, Ning , Li, Yan , Dai, Chengna et al. H2O in situ induced active site structure dynamics for efficient methane direct oxidation to methanol over Fe-BEA zeolite br [J]. | JOURNAL OF CATALYSIS , 2022 , 414 : 302-312 .
MLA Liu, Ning et al. "H2O in situ induced active site structure dynamics for efficient methane direct oxidation to methanol over Fe-BEA zeolite br" . | JOURNAL OF CATALYSIS 414 (2022) : 302-312 .
APA Liu, Ning , Li, Yan , Dai, Chengna , Xu, Ruinian , Yu, Gangqiang , Wang, Ning et al. H2O in situ induced active site structure dynamics for efficient methane direct oxidation to methanol over Fe-BEA zeolite br . | JOURNAL OF CATALYSIS , 2022 , 414 , 302-312 .
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Hafnium-tin composite oxides as effective synergistic catalysts for the conversion of glucose into 5-hydroxymethylfurfural SCIE
期刊论文 | 2022 , 311 | FUEL
WoS CC Cited Count: 20
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5-Hydroxymethylfurfural (5-HMF), an important and value-added platform chemical, has inspired increasing attention. In this study, hafnium-tin composite oxides (Sn-HfO2) were prepared by one-pot coprecipitation process and used as effective synergistic catalysts for 5-HMF synthesis from the conversion of glucose. Pyridine-FTIR results reveal that Sn-HfO2 catalysts have strong Lewis and weak Bronsted acid sites. With 0.5Sn-HfO2 as the catalyst, the highest yield of 5-HMF obtained from glucose was 75.5% with 99.5% conversion at 170 degrees C for 2 h in a methyl isobutyl ketone (MIBK)/water biphasic system. Furthermore, the catalytic system also possesses excellent performance in converting other carbohydrates. The catalysis mechanism for the isomerization of glucose to fructose was explored by the density functional theory (DFT) method, indicating that Lewis acidic Hf active sites and proton mediator Sn-O species synergistically catalyzed the isomerization process, effectively lowering the reaction energy barrier. The cooperative action of terminal Hf-OH and Sn-OH also facilitated the formation of 5-HMF in fructose dehydration. 0.5Sn-HfO2 could be reused for four runs without significant loss of catalytic activity. This approach provides the feasibility of composite oxides as synergistic catalysts for carbohydrate conversion to 5-HMF.

Keyword :

5-Hydroxymethylfurfural 5-Hydroxymethylfurfural Mechanism Mechanism Hafnium-tin composite oxides Hafnium-tin composite oxides Synergistic effect Synergistic effect Glucose Glucose

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GB/T 7714 Qiu, Guo , Chen, Biaohua , Liu, Ning et al. Hafnium-tin composite oxides as effective synergistic catalysts for the conversion of glucose into 5-hydroxymethylfurfural [J]. | FUEL , 2022 , 311 .
MLA Qiu, Guo et al. "Hafnium-tin composite oxides as effective synergistic catalysts for the conversion of glucose into 5-hydroxymethylfurfural" . | FUEL 311 (2022) .
APA Qiu, Guo , Chen, Biaohua , Liu, Ning , Huang, Chongpin . Hafnium-tin composite oxides as effective synergistic catalysts for the conversion of glucose into 5-hydroxymethylfurfural . | FUEL , 2022 , 311 .
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大型化工国有企业研究院所与高校合作构建创新团队的思考与实践
期刊论文 | 2022 , 51 (04) , 967-970 | 当代化工
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Abstract :

国有化工大型企业研究院所在化工生态文明建设中,以国家重大科研项目为载体,与高校组构建创新团队。以基础、应用基础为先导,构建知识、技术创新的平台,开发共性、关键技术,为行业科技进步服务,依靠现代化工技术,改造传统化工企业,建立新型化工产业。学科交叉的力度和广度是源头创新发展的关键性因素之一,团队带头人的作用、目标、运行的机制及其结构是创新团队的保障。

Keyword :

科技创新 科技创新 合作机制 合作机制 创新团队 创新团队

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GB/T 7714 王刚 , 张喜文 , 于晓方 et al. 大型化工国有企业研究院所与高校合作构建创新团队的思考与实践 [J]. | 当代化工 , 2022 , 51 (04) : 967-970 .
MLA 王刚 et al. "大型化工国有企业研究院所与高校合作构建创新团队的思考与实践" . | 当代化工 51 . 04 (2022) : 967-970 .
APA 王刚 , 张喜文 , 于晓方 , 刘建锟 , 王宁 , 陈标华 . 大型化工国有企业研究院所与高校合作构建创新团队的思考与实践 . | 当代化工 , 2022 , 51 (04) , 967-970 .
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咪唑基离子液体用于天然气脱水过程中的技术-环境评价
期刊论文 | 2022 , 40 (11) , 199-210 | 环境工程
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利用Aspen Plus建立离子液体天然气脱水的工艺流程模拟,结合灵敏度分析及生命周期评价方法,对该工艺应用不同离子液体产生的技术及环境影响进行比较,并分析离子液体结构对天然气脱水工艺技术及环境评价的影响.结果表明:与烷基链较短的阳离子结合的[BF4]-离子液体具有较好的脱水性能([EMIM][BF4]>[BMIM][BF4]>[OMIM][BF4]);对于生产1 kg甲烷气体而言,[BMIM][PF6]脱水法的环境影响最大,达到[OMIM][BF4]脱水法环境影响的5倍;此外,对于具有相同阴离子[BF4]-的脱水情况,环境影响顺序为[OMIM][BF4]<[BMIM][BF4]<[EMIM][BF4].该结果从技术和环境评价的角度为筛选或开发天然气脱水过程中选择适当的离子液体提供了指导.

Keyword :

离子液体 离子液体 能量分析 能量分析 过程模拟 过程模拟 天然气脱水 天然气脱水 生命周期评价 生命周期评价

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GB/T 7714 王佳琪 , 代成娜 , 于刚强 et al. 咪唑基离子液体用于天然气脱水过程中的技术-环境评价 [J]. | 环境工程 , 2022 , 40 (11) : 199-210 .
MLA 王佳琪 et al. "咪唑基离子液体用于天然气脱水过程中的技术-环境评价" . | 环境工程 40 . 11 (2022) : 199-210 .
APA 王佳琪 , 代成娜 , 于刚强 , 武斌 , 刘宁 , 徐瑞年 et al. 咪唑基离子液体用于天然气脱水过程中的技术-环境评价 . | 环境工程 , 2022 , 40 (11) , 199-210 .
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Innovative reactive distillation process for the eco-friendly Poly (oxymethylene) dimethyl ethers synthesis from methylal and trioxane SCIE
期刊论文 | 2022 , 278 | SEPARATION AND PURIFICATION TECHNOLOGY
WoS CC Cited Count: 11
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Poly(oxymethylene) dimethyl ethers (PODEn) is a promising excellent additive for diesel fuels. The PODEn production by traditional reactor conform to Schulz - Flory distribution resulting in low product yield and large circulating material flow, which leads to high energy consumption and cost. This study presents a novel reactive distillation (RD) process for the PODEn synthesis by polymerization reaction from trioxane and methylal. A rigorous simulation model of the RD process was developed for the plant design and scale-up. Also, a sensitivity analysis was performed to determine the influence of key operating parameters on the RD process performance. The production composition analysis indicates that the RD process can effectively control the degree of polymerization and obtain high selectivity for any target product(s). The techno-economic analysis shows that the process is feasible, with over 96% and 13% reduction in CapEx and OpEx, over 68% savings in total annual costs as compared to the reaction-separation technology. Higher conversion and selectivity can be obtained by RD, within lower recirculation rate (only 12281 kg/h instead of 2950 kg/h) as compared to the conventional process.

Keyword :

Process intensification Process intensification Process design Process design PODEn PODEn Reactive distillation Reactive distillation Methylal Methylal

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GB/T 7714 Meng, Ying , Li, Hong , Dai, Chengna et al. Innovative reactive distillation process for the eco-friendly Poly (oxymethylene) dimethyl ethers synthesis from methylal and trioxane [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2022 , 278 .
MLA Meng, Ying et al. "Innovative reactive distillation process for the eco-friendly Poly (oxymethylene) dimethyl ethers synthesis from methylal and trioxane" . | SEPARATION AND PURIFICATION TECHNOLOGY 278 (2022) .
APA Meng, Ying , Li, Hong , Dai, Chengna , Chen, Biaohua , Lei, Zhigang , Li, Xingang et al. Innovative reactive distillation process for the eco-friendly Poly (oxymethylene) dimethyl ethers synthesis from methylal and trioxane . | SEPARATION AND PURIFICATION TECHNOLOGY , 2022 , 278 .
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