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

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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Evaluation of activated sludge properties’ changes in industrial-wastewater pre-treatment: role of residual aluminum hydrolyzed species with different polymerization degree

《环境科学与工程前沿（英文）》 2023年 第17卷 第6期 doi: 10.1007/s11783-023-1675-3

摘要：

● Medium poly Al salts dominated the PAC residual salts with a rational dosage.

关键词： Coagulation/flocculation     Hydroxyl-aluminum     Hydrolysis reaction     Reactor performance     Activated sludge property     Surface properties    

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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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A perspective on the promoting effect of Ir and Au on Pd toward the ethanol oxidation reaction in alkaline

S. Y. SHEN, Y. G. GUO, G. H. WEI, L. X. LUO, F. LI, J. L. ZHANG

《能源前沿（英文）》 2018年 第12卷 第4期   页码 501-508 doi: 10.1007/s11708-018-0586-7

摘要： There remain great challenges in developing highly efficient electrocatalysts with both high activity and good stability for the ethanol oxidation reaction in alkaline media. Herein, two architectures of tri-metallic PdIrAu/C electrocatalysts are designed and the promoting effect of Au and Ir on Pd toward the ethanol oxidation reaction (EOR) in alkaline media is investigated in detail. On the one hand, the tri-metallic Pd Au Ir/C electrocatalyst with a solid solution alloy architecture is less active relative to Pd Ir/C and Pd/C while the stabilizing effect of Au leads to both a higher activity and a lower degradation percentage after 3000 cycles of the accelerated degradation test (ADT) on Pd Au Ir/C than those on Pd Ir/C. On the other hand, the tri-metallic Pd Ir@(1/3Au)/C electrocatalyst with a near surface alloy architecture delivers a much higher activity with an improvement up to 50.4% compared to Pd Ir/C. It is speculated that for the tri-metallic Pd Ir@(1/3Au)/C electrocatalyst, certain Au atoms are well designed on surfaces to introduce an electronic modification, thus leading to an anti-poisoning effect and improving the EOR activity.

关键词： fuel cells     catalysts     ethanol oxidation     alkaline media     solid solution alloy     near surface alloy    

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Cube-octameric silsesquioxane (POSS)-capped magnetic iron oxide nanoparticles for the efficient removal of methylene blue

Ali Akbari, Nasser Arsalani, Bagher Eftekhari-Sis, Mojtaba Amini, Gholamreza Gohari, Esmaiel Jabbari

《化学科学与工程前沿（英文）》 2019年 第13卷 第3期   页码 563-573 doi: 10.1007/s11705-018-1784-x

摘要： Octavinyl polyhedral oligomeric silsesquioxane (POSS) was polymerized on the surface of Fe O nanoparticles (NPs) and then the NPs were functionalized with carboxylic acid groups using thiol-ene click reactions with thioglycolic acid. The as-prepared Fe O @POSS-COOH magnetic hybrid NPs had mesoporous structures with an average particle diameter of 15 nm and a relatively high specific surface area of 447 m ∙g . Experimental results showed that 4 mg of Fe O @POSS-COOH NPs efficiently adsorbed and removed methylene blue from water at 5 min. This is due to the presence of both carboxylic acid and pendant vinyl groups on the Fe O @POSS-COOH NPs. These NPs could be easily withdrawn from water within a few seconds under moderate magnetic field and showed high stability in acid and alkaline aqueous mediums.

关键词： nanomagnetic POSS     surface polymerization     thiol-ene reaction     adsorbent     water treatment    

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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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Heterogeneous reaction mechanism of gaseous HNO

Nan ZHAO,Qingzhu ZHANG,Wenxing WANG

《环境科学与工程前沿（英文）》 2016年 第10卷 第5期 doi: 10.1007/s11783-016-0836-z

摘要： We studied the heterogeneous reaction mechanism of gaseous HNO with solid NaCl. HCl is released from heterogeneous reactions between gaseous HNO and solid NaCl. Water molecules induce surface reconstruction of NaCl to facilitate the reaction. Sea salt particles containing NaCl are among the most abundant particulate masses in coastal atmosphere. Reactions involving sea salt particles potentially generate Cl radicals, which are released into coastal atmosphere. Cl radicals play an important role in the nitrogen and O cycles, sulfur chemistry and particle formation in the troposphere of the polluted coastal regions. This paper aimed at the heterogeneous reaction between gaseous HNO and solid NaCl. The mechanism was investigated by density functional theory (DFT). The results imply that water molecules induce the surface reconstruction, which is essential for the heterogeneous reaction. The surface reconstruction on the defective (710) surface has a barrier of 10.24 kcal·mol and is endothermic by 9.69 kcal·mol , whereas the reconstruction on the clean (100) surface has a barrier of 18.46 kcal·mol and is endothermic by 12.96 kcal·mol . The surface reconstruction involved in water-adsorbed (710) surface is more energetically favorable. In comparison, water molecules adsorbed on NaCl (100) surface likely undergo water diffusion or desorption. Further, it reveals that the coordination number of the Cl is reduced after the surface reconstruction, which assists Cl to accept the proton from HNO . HCl is released from heterogeneous reactions between gaseous HNO and solid NaCl and can react with OH free radicals to produce atomic Cl radicals. The results will offer further insights into the impact of gaseous HNO on the air quality of the coastal areas.

关键词： Seasalt particles     NaCl     HNO3     Heterogeneous reaction     Reaction mechanism     Density functional theory    

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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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Graphene-reinforced metal-organic frameworks derived cobalt sulfide/carbon nanocomposites as efficient multifunctional electrocatalysts

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1487-1499 doi: 10.1007/s11705-021-2085-3

摘要： Developing cost-effective electrocatalysts for oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is vital in energy conversion and storage applications. Herein, we report a simple method for the synthesis of graphene-reinforced CoS/C nanocomposites and the evaluation of their electrocatalytic performance for typical electrocatalytic reactions. Nanocomposites of CoS embedded in N, S co-doped porous carbon and graphene (CoS@C/Graphene) were generated via simultaneous sulfurization and carbonization of one-pot synthesized graphite oxide-ZIF-67 precursors. The obtained CoS@C/Graphene nanocomposites were characterized by X-ray diffraction, Raman spectroscopy, thermogravimetric analysis-mass spectroscopy, scanning electronic microscopy, transmission electronic microscopy, X-ray photoelectron spectroscopy and gas sorption. It is found that CoS nanoparticles homogenously dispersed in the in situ formed N, S co-doped porous carbon/graphene matrix. The CoS@C/10Graphene composite not only shows excellent electrocatalytic activity toward ORR with high onset potential of 0.89 V, four-electron pathway and superior durability of maintaining 98% of current after continuously running for around 5 h, but also exhibits good performance for OER and HER, due to the improved electrical conductivity, increased catalytic active sites and connectivity between the electrocatalytic active CoS and the carbon matrix. This work offers a new approach for the development of novel multifunctional nanocomposites for the next generation of energy conversion and storage applications.

关键词： MOF derivative     graphene     electrocatalyst     oxygen reduction reaction     oxygen evolution reaction     hydrogen evolution reaction    

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Impact and inhibitory mechanism of phenolic compounds on the formation of toxic Maillard reaction products

Jing TENG, Xiaoqian HU, Ningping TAO, Mingfu WANG

《农业科学与工程前沿（英文）》 2018年 第5卷 第3期   页码 321-329 doi: 10.15302/J-FASE-2017182

摘要：

As one of the dominant reactions occurring during thermal treatment of food, the Maillard reaction not only leads to the formation of aroma, browning color and taste compounds, but also contributes to the formation of some unpleasant toxic substances including acrylamide, heterocyclic amines and advanced glycation end products. Polyphenols, one of the most abundant antioxidants in the human diet, are contained in different kinds of foods. In this review, some recent studies on the impact of dietary polyphenols on the formation of acrylamide, heterocyclic amines and advanced glycation end products formed during the Maillard reaction are summarized, including the research work conducted with both chemical model systems and real food model systems; the possible inhibitory mechanisms of different polyphenols are also summarized and discussed in this review. Basically we found that some dietary polyphenols not only scavenge free radicals, but also react with reactive carbonyl species, thus lowering the formation of toxic Maillard reaction products. This review provides a useful theoretical foundation for the application of polyphenols in food safety, and suggests some directions for further study of natural products as inhibitors against the formation of toxic substances in thermally processed food.

关键词： advanced glycation end products     acrylamide     food safety     heterocyclic amine     Maillard reaction     polyphenols    

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An overview and recent advances in electrocatalysts for direct seawater splitting

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1408-1426 doi: 10.1007/s11705-021-2102-6

摘要： In comparison to pure water, seawater is widely accepted as an unlimited resource. The direct seawater splitting is economical and eco-friendly, but the key challenges in seawater, especially the chlorine-related competing reactions at the anode, seriously hamper its practical application. The development of earth-abundant electrocatalysts toward direct seawater splitting has emerged as a promising strategy. Highly efficient electrocatalysts with improved selectivity and stability are of significance in preventing the interference of side reactions and resisting various impurities. This review first discusses the macroscopic understanding of direct seawater electrolysis and then focuses on the strategies for rational design of electrocatalysts toward direct seawater splitting. The perspectives of improved electrocatalysts to solve emerging challenges and further development of direct seawater splitting are also provided.

关键词： seawater splitting     electrocatalysts     oxygen evolution reaction     hydrogen evolution reaction     chlorine chemistry    

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Interface engineering for enhancing electrocatalytic oxygen evolution reaction of CoS/CeO heterostructures

《化学科学与工程前沿（英文）》 2022年 第16卷 第3期   页码 376-383 doi: 10.1007/s11705-021-2062-x

摘要： To realize renewable energy conversion, it is important to develop low-cost and high-efficiency electrocatalyst for oxygen evolution reaction. In this communication, a novel bijunction CoS/CeO2 electrocatalyst grown on carbon cloth is prepared by the interface engineering. The interface engineering of CoS and CeO2 facilitates a rapid charge transfer from CeO2 to CoS. Such an electrocatalyst exhibits outstanding electrocatalytic activity with a low overpotential of 311 mV at 10 mA∙cm−2 and low Tafel slope of 76.2 mV∙dec–1, and is superior to that of CoS (372 mV) and CeO2 (530 mV) counterparts. And it has long-term durability under alkaline media.

关键词： interface engineering     CoS/CeO2     electrodeposition     electrocatalyst     oxygen evolution reaction    

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Cell surface protein engineering for high-performance whole-cell catalysts

Hajime Nakatani,Katsutoshi Hori

《化学科学与工程前沿（英文）》 2017年 第11卷 第1期   页码 46-57 doi: 10.1007/s11705-017-1609-3

摘要： Cell surface protein engineering facilitated by accumulation of information on genome and protein structure involves heterologous production and modification of cell surface proteins using genetic engineering, and is important for the development of high-performance whole-cell catalysts. In this field, cell surface display is a major technology by exposing target proteins, such as enzymes, on the cell surface using a carrier protein. The target proteins are fused to the carrier proteins that transport and tether them to the cell surface, as well as to a secretion signal. This paper reviews cell surface display systems for prokaryotic and eukaryotic cells from the perspective of carrier proteins, which determine the number of displayed molecules, and the localization, size, and direction ( or terminal anchoring) of the passengers. We also discuss advanced methods for displaying multiple enzymes and a new method for the immobilization of whole-cell catalysts using adhesive surface proteins.

关键词： cell surface engineering     surface display     whole-cell catalysts     bioprocess    

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cluster-based organic frameworks as highly active electrocatalysts for oxygen reduction and oxygen evolution reaction

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 570-580 doi: 10.1007/s11705-022-2247-y

摘要： Recently, metal–organic frameworks are one of the potential catalytic materials for electrocatalytic applications. The oxygen reduction reaction and oxygen evolution reaction catalytic activities of heterometallic cluster-based organic frameworks are investigated using density functional theory. Firstly, the catalytic activities of heterometallic clusters are investigated. Among all heterometallic clusters, Fe2Mn–Mn has a minimum overpotential of 0.35 V for oxygen reduction reaction, and Fe2Co–Co possesses the smallest overpotential of 0.32 V for oxygen evolution reaction, respectively 100 and 50 mV lower than those of Pt(111) and RuO2(110) catalysts. The analysis of the potential gap of Fe2M clusters indicates that Fe2Mn, Fe2Co, and Fe2Ni clusters possess good bifunctional catalytic activity. Additionally, the catalytic activity of Fe2Mn and Fe2Co connected through 3,3′,5,5′-azobenzenetetracarboxylate linker to form Fe2M–PCN–Fe2M is explored. Compared with Fe2Mn–PCN–Fe2Mn, Fe2Co–PCN–Fe2Co, and isolated Fe2M clusters, the mixed-metal Fe2Co–PCN–Fe2Mn possesses excellent bifunctional catalytic activity, and the values of potential gap on the Mn and Co sites of Fe2Co–PCN–Fe2Mn are 0.69 and 0.70 V, respectively. Furthermore, the analysis of the electron structure indicates that constructing a mixed-metal cluster can efficiently enhance the electronic properties of the catalyst. In conclusion, the mixed-metal cluster strategy provides a new approach to further design and synthesize high-efficiency bifunctional electrocatalysts.

关键词： bimetallic metal–organic frameworks     bifunctional electrocatalyst     density functional theory     oxygen reduction reaction     oxygen evolution reaction    

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Polypyrrole@NiCo hybrid nanotube arrays as high performance electrocatalyst for hydrogen evolution reaction

Shenghua Ye, Gaoren Li

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 473-480 doi: 10.1007/s11705-018-1724-9

摘要：

The polypyrrole(PPy)@NiCo hybrid nanotube arrays have been successfully fabricated as a high performance electrocatalyst for hydrogen evolution reaction (HER) in alkaline solution. The strong electronic interactions between PPy and NiCo alloy are confirmed by X-ray photoelectron spectroscopy and Raman spectra. Because these interations can remarkably reduce the apparent activation energy (Ea) for HER and enhance the turnover frequency of catalysts, the electrocatalytic performance of PPy@NiCo hybrid nanotube arrays are significantly improved. The electrochemical tests show that the PPy@NiCo hybrid catalysts exhibit a low overpotential of ~186 mV at 10.0 mA·cm−2 and a small tafel slope of 88.6 mV·deg−1 for HER in the alkaline solution. The PPy@NiCo hybrid nanotubes also exhibit high catalytic activity and high stability for HER.

关键词： NiCo alloy     polypyrrole     hybrid nanotube     electrocatalyst     hydrogen evolution reaction    

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标题 作者 时间 类型 操作

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

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

期刊论文

Evaluation of activated sludge properties’ changes in industrial-wastewater pre-treatment: role of residual aluminum hydrolyzed species with different polymerization degree

期刊论文

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

期刊论文

A perspective on the promoting effect of Ir and Au on Pd toward the ethanol oxidation reaction in alkaline

S. Y. SHEN, Y. G. GUO, G. H. WEI, L. X. LUO, F. LI, J. L. ZHANG

期刊论文

Cube-octameric silsesquioxane (POSS)-capped magnetic iron oxide nanoparticles for the efficient removal of methylene blue

Ali Akbari, Nasser Arsalani, Bagher Eftekhari-Sis, Mojtaba Amini, Gholamreza Gohari, Esmaiel Jabbari

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

Heterogeneous reaction mechanism of gaseous HNO

Nan ZHAO,Qingzhu ZHANG,Wenxing WANG

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

Graphene-reinforced metal-organic frameworks derived cobalt sulfide/carbon nanocomposites as efficient multifunctional electrocatalysts

期刊论文

Impact and inhibitory mechanism of phenolic compounds on the formation of toxic Maillard reaction products

Jing TENG, Xiaoqian HU, Ningping TAO, Mingfu WANG

期刊论文

An overview and recent advances in electrocatalysts for direct seawater splitting

期刊论文

Interface engineering for enhancing electrocatalytic oxygen evolution reaction of CoS/CeO heterostructures

期刊论文

Cell surface protein engineering for high-performance whole-cell catalysts

Hajime Nakatani,Katsutoshi Hori

期刊论文

cluster-based organic frameworks as highly active electrocatalysts for oxygen reduction and oxygen evolution reaction

期刊论文

Polypyrrole@NiCo hybrid nanotube arrays as high performance electrocatalyst for hydrogen evolution reaction

Shenghua Ye, Gaoren Li

期刊论文