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Thermodynamic analysis of reaction pathways and equilibrium yields for catalytic pyrolysis of naphtha

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1700-1712 doi: 10.1007/s11705-022-2207-6

摘要： The chain length and hydrocarbon type significantly affect the production of light olefins during the catalytic pyrolysis of naphtha. Herein, for a better catalyst design and operation parameters optimization, the reaction pathways and equilibrium yields for the catalytic pyrolysis of C5–8 n/iso/cyclo-paraffins were analyzed thermodynamically. The results revealed that the thermodynamically favorable reaction pathways for n/iso-paraffins and cyclo-paraffins were the protolytic and hydrogen transfer cracking pathways, respectively. However, the formation of light paraffin severely limits the maximum selectivity toward light olefins. The dehydrogenation cracking pathway of n/iso-paraffins and the protolytic cracking pathway of cyclo-paraffins demonstrated significantly improved selectivity for light olefins. The results are thus useful as a direction for future catalyst improvements, facilitating superior reaction pathways to enhance light olefins. In addition, the equilibrium yield of light olefins increased with increasing the chain length, and the introduction of cyclo-paraffin inhibits the formation of light olefins. High temperatures and low pressures favor the formation of ethylene, and moderate temperatures and low pressures favor the formation of propylene. n-Hexane and cyclohexane mixtures gave maximum ethylene and propylene yield of approximately 49.90% and 55.77%, respectively. This work provides theoretical guidance for the development of superior catalysts and the selection of proper operation parameters for the catalytic pyrolysis of C5–8 n/iso/cyclo-paraffins from a thermodynamic point of view.

关键词： naphtha     catalytic pyrolysis     reaction pathway     equilibrium yield    

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Recent advances and challenges of nitrogen/nitrate electro catalytic reduction to ammonia synthesis

《能源前沿（英文）》 doi: 10.1007/s11708-023-0908-2

摘要： The Haber-Bosch process is the most widely used synthetic ammonia technology at present. Since its invention, it has provided an important guarantee for global food security. However, the traditional Haber-Bosch ammonia synthesis process consumes a lot of energy and causes serious environmental pollution. Under the serious pressure of energy and environment, a green, clean, and sustainable ammonia synthesis route is urgently needed. Electrochemical synthesis of ammonia is a green and mild new method for preparing ammonia, which can directly convert nitrogen or nitrate into ammonia using electricity driven by solar, wind, or water energy, without greenhouse gas and toxic gas emissions. Herein, the basic mechanism of the nitrogen reduction reaction (NRR) to ammonia and nitrate reduction reaction (NO3− RR) to ammonia were discussed. The representative approaches and major technologies, such as lithium mediated electrolysis and solid oxide electrolysis cell (SOEC) electrolysis for NRR, high activity catalyst and advanced electrochemical device fabrication for NO3 − RR and electrochemical ammonia synthesis were summarized. Based on the above discussion and analysis, the main challenges and development directions for electrochemical ammonia synthesis were further proposed.

关键词： electrochemical ammonia synthesis     nitrogen     nitrate     nitrogen reduction reaction (NRR) to ammonia     nitrate reduction reaction (NO–3 RR)    

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Dual-reaction-center catalytic process continues Fenton’s story

Chao Lu, Kanglan Deng, Chun Hu, Lai Lyu

《环境科学与工程前沿（英文）》 2020年 第14卷 第5期 doi: 10.1007/s11783-020-1261-x

摘要： Abstract • Dual-reaction-center (DRC) system breaks through bottleneck of Fenton reaction. • Utilization of intrinsic electrons of pollutants is realized in DRC system. • DRC catalytic process well continues Fenton’s story. Triggered by global water quality safety issues, the research on wastewater treatment and water purification technology has been greatly developed in recent years. The Fenton technology is particularly powerful due to the rapid attack on pollutants by the generated hydroxyl radicals (•OH). However, both heterogeneous and homogeneous Fenton/Fenton-like technologies follow the classical reaction mechanism, which depends on the oxidation and reduction of the transition metal ions at single sites. So even after a century of development, this reaction still suffers from its inherent bottlenecks in practical application. In recent years, our group has been focusing on studying a novel heterogeneous Fenton catalytic process, and we developed the dual-reaction-center (DRC) system for the first time. In the DRC system, H2O2 and O2 can be efficiently reduced to reactive oxygen species (ROS) in electron-rich centers, while pollutants are captured and oxidized by the electron-deficient centers. The obtained electrons from pollutants are diverted to the electron-rich centers through bonding bridges. This process breaks through the classic Fenton mechanism, and improves the performance and efficiency of pollutant removal in a wide pH range. Here, we provide a brief overview of Fenton’s story and focus on combing the discovery and development of the DRC technology and mechanism in recent years. The construction of the DRC and its performance in the pollutant degradation and interfacial reaction process are described in detail. We look forward to bringing a new perspective to continue Fenton’s story through research and development of DRC technology.

关键词： Dual reaction centers     Fenton     Pollutant utilization     Electron transfer    

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Effects of support acidity on the reaction mechanisms of selective catalytic reduction of NO by CH

Shicheng XU, Junhua LI, Dong YANG, Jiming HAO

《环境科学与工程前沿（英文）》 2009年 第3卷 第2期   页码 186-193 doi: 10.1007/s11783-009-0016-5

摘要： The reaction mechanisms of selective catalytic reduction (SCR) of nitric oxide (NO) by methane (CH ) over solid superacid-based catalysts were proposed and testified by DRIFTS studies on transient reaction as well as by kinetic models. Catalysts derived from different supports would lead to different reaction pathways, and the acidity of solid superacid played an important role in determining the reaction mechanisms and the catalytic activities. Higher ratios of Br?nsted acid sites to Lewis acid sites would lead to stronger oxidation of methane and then could facilitate the step of methane activation. Strong Br?nsted acid sites would not necessarily lead to better catalytic performance, however, since the active surface NO species and the corresponding reaction routes were determined by the overall acidity strength of the support. The reaction routes where NO moiety was engaged as an important intermediate involved moderate oxidation of methane, the rate of which could determine the overall activity. The reaction involving NO moiety was likely to be determined by the step of reduction of NO. Therefore, to enhance the SCR activity of solid superacid catalysts, reactions between appropriate couples of active NO species and activated hydrocarbon intermediates should be realized by modification of the support acidity.

关键词： selective catalytic reduction (SCR)     nitric oxide (NO)     methane     support acidity     Br?nsted acid sites     NOy species    

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Probing the catalytic activity of M-N

Fan Ge, Qingan Qiao, Xin Chen, You Wu

《化学科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 1206-1216 doi: 10.1007/s11705-020-2017-7

摘要： In this work, the detailed oxygen reduction reaction (ORR) catalytic performance of M-N O (M= Fe, Co, and Ni; = 1–4) has been explored via the detailed density functional theory method. The results suggest that the formation energy of M-N O shows a good linear relationship with the number of doped O atoms. The adsorption manner of O on M-N O changed from end-on ( = 1 and 2) to side-on ( = 3 and 4), and the adsorption strength gradually increased. Based on the results for binding strength of ORR intermediates and the Gibbs free energy of ORR steps on the studied catalysts, we screened out two highly active ORR catalysts, namely Co-N O and Ni-N O , which possess very small overpotentials of 0.27 and 0.32 V, respectively. Such activities are higher than the precious Pt catalyst. Electronic structure analysis reveals one of the reasons for the higher activity of Co-N O and Ni-N O is that they have small energy gaps and moderate highest occupied molecular orbital energy levels. Furthermore, the results of the density of states reveal that the O doping can improve the electronic structure of the original catalyst to tune the adsorption of the ORR intermediates.

关键词： M-N-C catalyst     oxygen doping     oxygen reduction reaction     catalytic activity     density functional theory    

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Hydrogen production by catalytic gasification of cellulose in supercritical water

GUAN Yu, PEI Aixia, GUO Liejin

《化学科学与工程前沿（英文）》 2008年 第2卷 第2期   页码 176-180 doi: 10.1007/s11705-008-0026-z

摘要： Cellulose, one of the important components of biomass, was gasified in supercritical water to produce hydrogen-rich gas in an autoclave which was operated batch-wise under high-pressure. KCO and Ca(OH) were selected as the catalysts (or promoters). The temperature was kept between 450°C and 500°C while pressure was maintained at 24–26 MPa. The reaction time was 20 min. Experimental results showed that the two catalysts had good catalytic effect and optimum amounts were observed for each catalyst. When 0.2 g KCO was added, the hydrogen yield could reach 9.456 molkg which was two times of the H amount produced without catalyst. When 1.6 g Ca(OH) was added, the H yield was 8.265 molkg which is lower than that obtained using KCO as catalyst but is still 1.7 times that achieved without catalyst. Comparing with the results obtained using KCO or Ca(OH) alone, the use of a combination of KCO and Ca(OH) could increase the H yield by up to 2.5 times that without catalyst and 25% and 45% more than that obtained using KCO and Ca(OH) alone, respectively. It was found that methane was the dominant product at relatively low temperature. When the temperature was increased, the methane reacts with water and is converted to hydrogen and carbon dioxide.

关键词： reaction     temperature     combination     catalytic effect     dominant product    

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Effect of alkyl nitrite decomposition on catalytic performance of CO coupling reaction over supported

Zhenhua LI, Weihan WANG, Dongxue YIN, Jing LV, Xinbin MA

《化学科学与工程前沿（英文）》 2012年 第6卷 第4期   页码 410-414 doi: 10.1007/s11705-012-1213-5

摘要： The syntheses of dimethyl oxalate (DMO) and diethyl oxalate (DEO) by CO coupling reaction in gaseous phase were investigated in a fixed bed reactor over Pd-Fe/Al O catalyst. The catalytic performance was characterized by CO conversion, space-time yield (STY) and selectivity of DMO (or DEO). The results showed that over Pd-Fe/Al O catalyst, the STY of DMO was higher than that of DEO under the same reaction conditions. The optimum reaction temperatures for synthesizing DMO and DEO were 403 K and 393 K, respectively, at the molar ratio 1 ∶ 1 of alkyl nitrite to CO. The difference in synthesizing DMO and DEO on the same catalyst was attributed to the decomposition performances of methyl nitrite (MN) and ethyl nitrite (EN), as density functional theory (DFT) calculation showed that EN decomposed more easily than MN.

关键词： palladium     CO coupling     dialkyl oxalate     alkyl nitrite     decomposition    

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Isolation of microbe for asymmetric reduction of prochiral aromatic ketone and its reaction characters

YANG Zhonghua, WANG Yu, WANG Guanghui, ZENG Rong, YAO Shanjing

《化学科学与工程前沿（英文）》 2007年 第1卷 第4期   页码 416-420 doi: 10.1007/s11705-007-0076-7

摘要： The favorable microbes for the asymmetric reduction of prochiral aromatic ketones was isolated from soil using acetophenone as the sole carbon source, when the asymmetric reduction of acetophenone (ACP) to chiral ?-phenethyl alcohol (PEA) was chosen as the model reaction. Two microbe strains with excellent catalytic activity were obtained. They were and identified by bacteria identification. The product of the asymmetric reduction of ACP catalyzed by was mainly R-PEA and that by was mainly S-PEA. The yield and enantiomeric excesses (e.e.) could respectively reach 75% and 90% for , and 80% and 70% for , much higher than those catalyzed by baker s yeast.

关键词： excellent catalytic     prochiral aromatic     enantiomeric     -phenethyl     catalytic activity    

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催化裂化过程反应化学的进展

许友好,汪燮卿

《中国工程科学》 2007年 第9卷 第8期   页码 6-14

摘要：

面对催化裂化工艺所遇到的挑战，提出了催化裂化过程反应化学的多维反应结构模式。多维反应结构模式的建立是基于对烃类在酸性催化剂上反应化学认识而进行的知识创新，但多维反应结构不同于烃类在酸性催化剂上反应化学。具有多维反应结构的催化裂化工艺更具有多样性和灵活性，基于此已成功地开发了多产异构烷烃的催化裂化工艺和生产清洁汽油和多产丙烯的催化裂化工艺。

关键词： 催化裂化     反应化学     催化剂     多维反应结构     两个反应区    

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Catalytic combustion of volatile organic compounds using perovskite oxides catalysts—a review

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1649-1676 doi: 10.1007/s11705-023-2324-x

摘要： With the rapid development of industry, volatile organic compounds (VOCs) are gaining attention as a class of pollutants that need to be eliminated due to their adverse effects on the environment and human health. Catalytic combustion is the most popular technology used for the removal of VOCs as it can be adapted to different organic emissions under mild conditions. This review first introduces the hazards of VOCs, their treatment technologies, and summarizes the treatment mechanism issues. Next, the characteristics and catalytic performance of perovskite oxides as catalysts for VOC removal are expounded, with a special focus on lattice distortions and surface defects caused by metal doping and surface modifications, and on the treatment of different VOCs. The challenges and the prospects regarding the design of perovskite oxides catalysts for the catalytic combustion of VOCs are also discussed. This review provides a reference base for improving the performance of perovskite catalysts to treat VOCs.

关键词： perovskite oxides     volatile organic compounds     catalytic combustion     reaction mechanism    

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production from co-gasification of coal and biomass in supercritical water by continuous flow thermal-catalyticreaction system

YAN Qiuhui, GUO Liejin, LIANG Xing, ZHANG Ximin

《能源前沿（英文）》 2007年 第1卷 第3期   页码 327-330 doi: 10.1007/s11708-007-0048-0

摘要： Hydrogen is a clean energy carrier. Converting abundant coal sources and green biomass energy into hydrogen effectively and without any pollution promotes environmental protection. The co-gasification performance of coal and a model compound of biomass, carboxymethylcellulose (CMC) in supercritical water (SCW), were investigated experimentally. The influences of temperature, pressure and concentration on hydrogen production from co-gasification of coal and CMC in SCW under the given conditions (20–25 MPa, 650vH, 15–30 s) are discussed in detail. The experimental results show that H, CO and CH are the main gas products, and the molar fraction of hydrogen reaches in excess of 60%. The higher pressure and higher CMC content facilitate hydrogen production; production is decreased remarkably given a longer residence time.

关键词： carboxymethylcellulose     temperature     co-gasification performance     Hydrogen     residence    

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Experimental research on catalysts and their catalytic mechanism for hydrogen production by gasification

PEI Aixia, GUO Liejin, JIN Hui

《能源前沿（英文）》 2007年 第1卷 第4期   页码 451-456 doi: 10.1007/s11708-007-0066-2

摘要： Peanut shell, mixed with sodium carboxymethylcellulose, was gasified at a temperature of 450°C and a pressure range from 24 to 27 MPa with the presence of different catalysts, including KCO, ZnCl and Raney-Ni. The experimental results show that different catalysts have greatly different effects on the reaction. Gasification efficiency (GE), hydrogen gasification efficiency (GHE), carbon gasification efficiency (GCE), yield of hydrogen production ( ) and potential yield of hydrogen production () are applied to describe the catalytic efficiency. From the result of gaseous components, ZnCl has the highest hydrogen selectivity, KCO is lower, and Raney-Ni is the lowest, but Raney-Ni is the most favorable to gasify biomass among the three catalysts, and its , , reach 126.84%, 185.71%, 94.24%, respectively. As expected, hydrogen selectivity increased and CH reduced rapidly when the mixture of ZnCl and Raney-Ni is used under the same condition. The optimization mixture appeared when 0.2 g of ZnCl was added to 1 g of Raney-Ni, 43.56 g · kg of hydrogen pro duction was obtained. In addition, the catalytic mechanisms of different catalysts were analyzed, and the possible reaction pathway was brought forward, which helped to explain the experiment phenomena and results correctly.

关键词： presence     Raney-Ni     biomass     optimization mixture     possible reaction    

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Significant enhancement in catalytic ozonationefficacy: From granular to super-fine powdered activated

Tianyi Chen, Wancong Gu, Gen Li, Qiuying Wang, Peng Liang, Xiaoyuan Zhang, Xia Huang

《环境科学与工程前沿（英文）》 2018年 第12卷 第1期 doi: 10.1007/s11783-018-1022-2

摘要： In this study, super-fine powdered activated carbon (SPAC) hasbeen proposed and investigated as a novel catalyst for the catalyticozonation of oxalate for the first time. SPAC was prepared from commercialgranular activated carbon (GAC) by ball milling. SPAC exhibited highexternal surface area with a far greater member of meso- and macropores(563% increase in volume). The catalytic performances of activatedcarbons (ACs) of 8 sizes were compared and the rate constant for pseudofirst-order total organic carbon removal increased from 0.012 min to 0.568 min (47-fold increase) withthe decrease in size of AC from 20 to 40 mesh (863 mm) to SPAC (~1.0 mm). Furthermore, the diffusion resistance of SPAC decreased17-fold compared with GAC. The ratio of oxalate degradation by surfacereaction increased by 57%. The rate of transformationof ozone to radicals by SPAC was 330 times that of GAC. The resultssuggest that a series of changes stimulated by ball milling, includinga larger ratio of external surface area, less diffusion resistance,significant surface reaction and potential oxidized surface all contributedto enhancing catalytic ozonation performance. This study demonstratedthat SPAC is a simple and effective catalyst for enhancing catalyticozonation efficacy.

关键词： Super-fine activated carbon     Catalytic ozonation     External surface area     Surface reaction     Hydroxyl radical    

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Catalytic activity of noble metal nanoparticles toward hydrodechlorination: influence of catalyst electronic

Man ZHANG,Feng HE,Dongye ZHAO

《环境科学与工程前沿（英文）》 2015年 第9卷 第5期   页码 888-896 doi: 10.1007/s11783-015-0774-1

摘要： In this study, stabilized Pd, Pt and Au nanoparticles were successfully prepared in aqueous phase using sodium carboxymethyl cellulose (CMC) as a capping agent. These metal nanoparticles were then tested for catalytic hydrodechlorination toward two classes of organochlorinated compounds (vinyl polychlorides including trichloroethylene (TCE), tetrachloroethylene (PCE), and alkyl polychlorides including 1,1,1-trichloroethane (1,1,1-TCA), and 1,1,1,2-tetrachloroethane (1,1,1,2-TeCA)) to determine the rate-limiting steps and to explore the reaction mechanisms. The surface area normalized reaction rate constant, , showed a systematic dependence on the electronic structure (the density of states at the Fermi level) of the metals, suggesting that adsorption of organochlorinated reactants on the metal catalyst surfaces is the rate-limiting step for catalytic hydrodechlorination. Hydrodechlorination rates of 1,1,1-TCA and 1,1,1,2-TeCA agreed with the bond strength of the first (weakest) dissociated C-Cl bond, suggesting that C-Cl bond cleavage, which is the first step for dissociative adsorption of the alkyl polychlorides, controlled the catalytic hydrodechlorination rate. However, hydrodechlorination rates of TCE and PCE correlated with the adsorption energies of their molecular (non-dissociative) adsorption on the noble metals rather than with the first C-Cl bond strength, suggesting that molecular adsorption governs the reaction rate for hydrodechlorination of the vinyl polychlorides.

关键词： catalytic hydrodechlorination     electronic structure     metal nanoparticles     reaction mechanisms    

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An investigation of reaction furnace temperatures and sulfur recovery

S. ASADI, M. PAKIZEH, M. POURAFSHARI CHENAR

《化学科学与工程前沿（英文）》 2011年 第5卷 第3期   页码 362-371 doi: 10.1007/s11705-011-1106-z

摘要： In a modern day sulfur recovery unit (SRU), hydrogen sulfide (H S) is converted to elemental sulfur using a modified Claus unit. A process simulator called TSWEET has been used to consider the Claus process. The effect of the H S concentration, the H S/CO ratio, the input air flow rate, the acid gas flow of the acid gas (AG) splitter and the temperature of the acid gas feed at three different oxygen concentrations (in the air input) on the main burner temperature have been studied. Also the effects of the tail gas ratio and the catalytic bed type on the sulfur recovery were studied. The bed temperatures were optimized in order to enhance the sulfur recovery for a given acid gas feed and air input. Initially when the fraction of AG splitter flow to the main burner was increased, the temperature of the main burner increased to a maximum but then decreased sharply when the flow fraction was further increased; this was true for all three concentrations of oxygen. However, if three other parameters (the concentration of H S, the ratio H S/CO and the flow rate of air) were increased, the temperature of the main burner increased monotonically. This increase had different slopes depending on the oxygen concentration in the input air. But, by increasing the temperature of the acid gas feed, the temperature of the main burner decreased. In general, the concentration of oxygen in the input air into the Claus unit had little effect on the temperature of the main burner (This is true for all parameters). The optimal catalytic bed temperature, tail gas ratio and type of catalytic bed were also determined and these conditions are a minimum temperature of 300°C, a ratio of 2.0 and a hydrolysing Claus bed.

关键词： Claus unit     concentration of H2S     tail gas ratio     sulfur recovery     catalytic bed    

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标题 作者 时间 类型 操作

Thermodynamic analysis of reaction pathways and equilibrium yields for catalytic pyrolysis of naphtha

期刊论文

Recent advances and challenges of nitrogen/nitrate electro catalytic reduction to ammonia synthesis

期刊论文

Dual-reaction-center catalytic process continues Fenton’s story

Chao Lu, Kanglan Deng, Chun Hu, Lai Lyu

期刊论文

Effects of support acidity on the reaction mechanisms of selective catalytic reduction of NO by CH

Shicheng XU, Junhua LI, Dong YANG, Jiming HAO

期刊论文

Probing the catalytic activity of M-N

Fan Ge, Qingan Qiao, Xin Chen, You Wu

期刊论文

Hydrogen production by catalytic gasification of cellulose in supercritical water

GUAN Yu, PEI Aixia, GUO Liejin

期刊论文

Effect of alkyl nitrite decomposition on catalytic performance of CO coupling reaction over supported

Zhenhua LI, Weihan WANG, Dongxue YIN, Jing LV, Xinbin MA

期刊论文

Isolation of microbe for asymmetric reduction of prochiral aromatic ketone and its reaction characters

YANG Zhonghua, WANG Yu, WANG Guanghui, ZENG Rong, YAO Shanjing

期刊论文

催化裂化过程反应化学的进展

许友好,汪燮卿

期刊论文

Catalytic combustion of volatile organic compounds using perovskite oxides catalysts—a review

期刊论文

production from co-gasification of coal and biomass in supercritical water by continuous flow thermal-catalyticreaction system

YAN Qiuhui, GUO Liejin, LIANG Xing, ZHANG Ximin

期刊论文

Experimental research on catalysts and their catalytic mechanism for hydrogen production by gasification

PEI Aixia, GUO Liejin, JIN Hui

期刊论文

Significant enhancement in catalytic ozonationefficacy: From granular to super-fine powdered activated

Tianyi Chen, Wancong Gu, Gen Li, Qiuying Wang, Peng Liang, Xiaoyuan Zhang, Xia Huang

期刊论文

Catalytic activity of noble metal nanoparticles toward hydrodechlorination: influence of catalyst electronic

Man ZHANG,Feng HE,Dongye ZHAO

期刊论文

An investigation of reaction furnace temperatures and sulfur recovery

S. ASADI, M. PAKIZEH, M. POURAFSHARI CHENAR

期刊论文