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The catalytic effect of both oxygen-bearing functional group and ash in carbonaceous catalyst on CH 4

Weidong ZHANG, Yongfa ZHANG,

《化学科学与工程前沿（英文）》 2010年 第4卷 第2期   页码 147-152 doi: 10.1007/s11705-009-0242-1

摘要： A kind of new catalyst—carbonaceous catalyst—for CH-CO reformation has been developed in our laboratory. The effect of both oxygen-bearing functional group such as phenolic hydroxyl, carbonyl, carboxyl, and lactonic, and ash such as FeO, NaCO, and KCO in the carbonaceous catalyst on the CH-CO reforming has been investigated with a fixed-bed reactor. It has been found that the carbonaceous catalyst is an efficient catalyst on CO-CH reforming. With the decrease of oxygen-bearing functional group, the catalytic activity of carbonaceous catalyst decreases quickly. The oxygen-bearing functional groups play a significant role in the carbonaceous-catalyzed CO-CH reforming; the ash components in carbonaceous catalyst also have an important influence on the CO-CH reforming. FeO, NaCO, and KCO in the ash can catalyze the CO-CH reforming reaction; CaO has little effect on CO-CH reforming reaction. CaO can catalyze the gasification between carbonaceous catalyst and CO; AlO and MgO inhibit the CO-CH reforming.

关键词： oxygen-bearing functional     carboxyl     phenolic hydroxyl     CH-CO reformation     CO-CH reforming    

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Effect of carbon deposition over carbonaceous catalysts on CH

Yongfa ZHANG, Meng ZHANG, Guojie ZHANG, Huirong ZHANG

《化学科学与工程前沿（英文）》 2010年 第4卷 第4期   页码 481-485 doi: 10.1007/s11705-010-0523-8

摘要： An investigation was made using a continuous fixed bed reactor to understand the influence of carbon deposition obtained under different conditions on CH -CO reforming. Thermogravimetry (TG) and X-ray diffraction (XRD) were employed to study the characteristics of carbon deposition. It was found that the carbonaceous catalyst is an efficient catalyst in methane decomposition and CH -CO reforming. The trend of methane decomposition at lower temperatures is similar to that at higher temperatures. The methane conversion is high during the initial of stage of the reaction, and then decays to a relatively fixed value after about 30 min. With temperature increase, the methane decomposition rate increases quickly. The reaction temperature has significant influence on methane decomposition, whereas the carbon deposition does not affect methane decomposition significantly. Different types of carbon deposition were formed at different methane decomposition reaction temperatures. The carbon deposition Type I generated at 900°C has a minor effect on CH -CO reforming and it easily reacts with carbon dioxide, but the carbon deposition Type II generated at 1000°C and 1100°C clearly inhibits CH -CO reforming and it is difficult to react with carbon dioxide. The results of XRD showed that some graphite structures were found in carbon deposition Type II.

关键词： carbon deposition     carbonaceous catalyst     CH4-CO2 reforming    

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Synthesis of magnetic carbonaceous acid derived from waste garlic peel for biodiesel production via esterification

Hewei YU, Jinke WU, Wei WEI, Xingyu ZHANG, Changzai REN, Yaoqi DONG, Shen CHENG

《能源前沿（英文）》 2023年 第17卷 第1期   页码 176-187 doi: 10.1007/s11708-022-0836-6

摘要： Waste biomass-supported magnetic solid acids have particular advantages in catalyst separation. First, a novel magnetic carbonaceous catalyst was synthesized from waste garlic peel (GP) via in situ impregnation before conducting carbonization at 450–600°C and sulfonation at 105°C. The physical and chemical properties of the synthesized catalysts were characterized. It was found that the magnetism of the catalyst increased with the carbonization temperature. The optimized catalyst, carbonized at 600°C (C600-S), possessed an excellent magnetization value of 12.5 emu/g, with a specific surface area of 175.1 m2/g, a pore volume of 0.16 cm3/g, and an acidic property of 0.74 mmol/g -SO3H density. By optimizing the esterification conditions to produce biodiesel, an oleic acid conversion of 94.5% was achieved at w(catalyst dosage) = 10% (w is mass fraction), a molar ratio of n(methanol): n(oleic acid) = 10: 1 (n is the amount of substance), and a reaction for 4 h at 90°C. Further, for catalyst regeneration, it was found that sulfuric acid treatment was more effective for improving the esterification activity than solvent washing, with which a conversion of more than 76% was achieved after the third run.

关键词： garlic peel (GP)     magnetic carbonaceous acid     esterification     biodiesel    

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Reactivity of Pyrogenic Carbonaceous Matter (PCM) in mediating environmental reactions: Current knowledge

Wenqing Xu, Mark L. Segall, Zhao Li

《环境科学与工程前沿（英文）》 2020年 第14卷 第5期 doi: 10.1007/s11783-020-1265-6

摘要： Abstract • Pyrogenic Carbonaceous Matter (PCM) promote both chemical and microbial synergies. • Discussion of PCM-enhanced abiotic transformation pathways of organic pollutants. • Conjugated microporous polymers (CMPs) can mimic the performance of PCM. • CMPs offer a platform that allows for systematic variation of individual properties. Pyrogenic Carbonaceous matter (PCM; e.g., black carbon, biochar, and activated carbon) are solid residues from incomplete combustion of fossil fuel or biomass. They are traditionally viewed as inert adsorbents for sequestering contaminants from the aqueous phase or providing surfaces for microbes to grow. In this account, we reviewed the recently discovered reactivity of PCM in promoting both chemical and microbial synergies that are important in pollutant transformation, biogeochemical processes of redox-active elements, and climate change mitigation with respect to the interaction between biochar and nitrous oxide (N2O). Moreover, we focused on our group’s work in the PCM-enhanced abiotic transformation of nitrogenous and halogenated pollutants and conducted in-depth analysis of the reaction pathways. To understand what properties of PCM confer its reactivity, our group pioneered the use of PCM-like polymers, namely conjugated microporous polymers (CMPs), to mimic the performance of PCM. This approach allows for the controlled incorporation of specific surface properties (e.g., quinones) into the polymer network during the polymer synthesis. As a result, the relationship between specific characteristics of PCM and its reactivity in facilitating the decay of a model pollutant was systematically studied in our group’s work. The findings summarized in this account help us to better understand an overlooked environmental process where PCM synergistically interacts with various environmental reagents such as hydrogen sulfide and water. Moreover, the knowledge gained in these studies could inform the design of a new generation of reactive carbonaceous materials with tailored properties that are highly efficient in contaminant removal.

关键词： pyrogenic carbonaceous matter     Conjugated microporous polymer     remediation     Biochar     Hydrolysis     Pollutant degradation    

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Emission factors of gaseous carbonaceous species from residential combustion of coal and crop residue

Qin WANG, Chunmei GENG, Sihua LU, Wentai CHEN, Min SHAO

《环境科学与工程前沿（英文）》 2013年 第7卷 第1期   页码 66-76 doi: 10.1007/s11783-012-0428-5

摘要： Experiments were performed to measure the emission factors ( s) of gaseous carbonaceous species, such as CO , CO, CH , and non-methane volatile organic compounds (NMVOCs), from the combustion of five types of coal of varying organic maturity and two types of biomass briquettes under residential burning conditions. Samples were collected in stainless steel canisters and 2,4-dinitrophenylhydrazine (DNPH) cartridges and were analyzed by GC–FID/MS and HPLC, respectively. The s from crop residue briquette burning were generally higher than those from coals, with the exception of CO . The dominant NMVOC species identified in coal smoke were carbonyls (41.7%), followed by C2 unsaturated hydrocarbons (29.1%) and aromatics (12.1%), while C2 unsaturated hydrocarbons were the dominant species (68.9%) emitted from the combustion of crop residue briquettes, followed by aromatics (14.4%). A comparison of burning normal crop residues in stoves and the open field indicated that briquettes emitted a larger proportion of ethene and acetylene. Both combustion efficiency and coal organic maturity had a significant impact on NMVOC s from burning coal: NMVOC emissions increased with increasing coal organic maturity but decreased as the combustion efficiency improved. Emissions from the combustion of crop residue briquettes from stoves occurred mainly during the smoldering process, with low combustion efficiency. Therefore, an improved stove design to allow higher combustion efficiency would be beneficial for reducing emissions of carbonaceous air pollutants.

关键词： residential combustion     coal     crop residue briquette     emission factors     gaseous carbonaceous species    

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Interaction of carbonaceous nanomaterials with wastewater biomass

Yu YANG,Zhicheng YU,Takayuki NOSAKA,Kyle DOUDRICK,Kiril HRISTOVSKI,Pierre HERCKES,Paul WESTERHOFF

《环境科学与工程前沿（英文）》 2015年 第9卷 第5期   页码 823-831 doi: 10.1007/s11783-015-0787-9

摘要： Increasing production and use of carbonaceous nanomaterials (NMs) will increase their release to the sewer system and to municipal wastewater treatment plants. There is little quantitative knowledge on the removal of multi-walled carbon nanotubes (MWCNTs), graphene oxide (GO), or few-layer graphene (FLG) from wastewater into the wastewater biomass. As such, we investigated the quantification of GO and MWCNTs by UV-Vis spectrophotometry, and FLG using programmable thermal analysis (PTA), respectively. We further explored the removal of pristine and oxidized MWCNTs (O-MWCNTs), GO, and FLG in a biomass suspension. At least 96% of pristine and O-MWCNTs were removed from the water phase through aggregation and 30-min settling in presence or absence of biomass with an initial MWCNT concentration of 25 mg·L . Only 65% of GO was removed with biomass concentration at or above 1,000 mg·L as total suspended solids (TSS) with the initial GO concentration of 25 mg·L . As UV-Vis spectrophotometry does not work well on quantification of FLG, we studied the removal of FLG at a lower biomass concentration (50 mg TSS·L ) using PTA, which showed a 16% removal of FLG with an initial concentration of 1 mg·L . The removal data for GO and FLG were fitted using the Freundlich equation ( = 0.55, 0.94, respectively). The data presented in this study for carbonaceous NM removal from wastewater provides quantitative information for environmental exposure modeling and life cycle assessment.

关键词： multi-walled carbon nanotubes     graphene oxide     graphene     removal     wastewater biomass    

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Modeling nanostructured catalyst layer in PEMFC and catalyst utilization

Jiejing ZHANG, Pengzhen CAO, Li XU, Yuxin WANG

《化学科学与工程前沿（英文）》 2011年 第5卷 第3期   页码 297-302 doi: 10.1007/s11705-011-1201-1

摘要： A lattice model of the nanoscaled catalyst layer structure in proton exchange membrane fuel cells (PEMFC) was established by Monte Carlo method. The model takes into account all the four components in a typical PEMFC catalyst layer: platinum (Pt), carbon, ionomer and pore. The elemental voxels in the lattice were set fine enough so that each average sized Pt particulate in Pt/C catalyst can be represented. Catalyst utilization in the modeled catalyst layer was calculated by counting up the number of facets of Pt voxels where “three phase contact” are met. The effects of some factors, including porosity, ionomer content, Pt/C particle size and Pt weight percentage in the Pt/C catalyst, on catalyst utilization were investigated and discussed.

关键词： catalyst layer     PEM fuel cell     lattice model     Monte Carlo method     catalyst utilization    

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Oxidant or catalyst for oxidation?

Jianzhi Huang, Huichun Zhang

《环境科学与工程前沿（英文）》 2019年 第13卷 第5期 doi: 10.1007/s11783-019-1158-8

摘要： Manganese oxides (MnOx) have been demonstrated to be effective materials to activate Oxone (i.e., PMS) to degrade various contaminants. However, the contribution of direct oxidation by MnOx to the total contaminant degradation under acidic conditions was often neglected in the published work, which has resulted in different and even conflicting interpretations of the reaction mechanisms. Here, the role of MnOx (as both oxidants and catalysts) in the activation of Oxone was briefly discussed. The findings offered new insights into the reaction mechanisms in PMS-MnOx and provided a more accurate approach to examine contaminant degradation for water/wastewater treatment.

关键词： Peroxymonosulfate     Manganese oxides     Catalyst     Oxidant    

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Monte Carlo simulation of the PEMFC catalyst layer

WANG Hongxing, CAO Pengzhen, WANG Yuxin

《化学科学与工程前沿（英文）》 2007年 第1卷 第2期   页码 146-150 doi: 10.1007/s11705-007-0027-3

摘要： The performance of the polymer electrolyte membrane fuel cell (PEMFC) is greatly controlled by the structure of the catalyst layer. Low catalyst utilization is still a significant obstacle to the commercialization of the PEMFC. In order to get a fundamental understanding of the electrode structure and to find the limiting factor in the low catalyst utilization, it is necessary to develop the mechanical model on the effect of catalyst layer structure on the catalyst utilization and the performance of the PEMFC. In this work, the structure of the catalyst layer is studied based on the lattice model with the Monte Carlo simulation. The model can predict the effects of some catalyst layer components, such as Pt/C catalyst, electrolyte and gas pores, on the utilization of the catalyst and the cell performance. The simulation result shows that the aggregation of conduction grains can greatly affect the degree of catalyst utilization. The better the dispersion of the conduction grains, the larger the total effective area of the catalyst is. To achieve higher utilization, catalyst layer components must be distributed by means of engineered design, which can prevent aggregation.

关键词： catalyst utilization     PEMFC     commercialization     Pt/C catalyst     conduction    

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Dendritic BiVO4 decorated with MnOx co-catalyst as an efficient hierarchical catalyst for photocatalytic

Jin Yang, Xuelian Liu, Hongbin Cao, Yanchun Shi, Yongbing Xie, Jiadong Xiao

《化学科学与工程前沿（英文）》 2019年 第13卷 第1期   页码 185-191 doi: 10.1007/s11705-018-1713-z

摘要： An appropriate co-catalyst can significantly promote the photocatalytic efficacy, but this has been seldom studied in the visible-light photocatalysis combined with ozone, namely photocatalytic ozonation. In this work, a dendritic bismuth vanadium tetraoxide (BiVO ) material composited with highly dispersed MnO nanoparticles was synthesized, and its catalytic activity is 86.6% higher than bare BiVO in a visible light and ozone combined process. Catalytic ozonation experiments, ultra-violet-visible (UV-Vis) diffuse reflectance spectra and photoluminescence spectra jointly indicate that MnO plays a triple role in this process. MnO strengthens the light adsorption and promotes the charge separation on the composite material, and it also shows good activity in catalytic ozonation. The key reactive species in this process is ·OH, and various pathways for its generation in this process is proposed. This work provides a new direction of catalyst preparation and pushes forward the application of photocatalytic ozonation in water treatment.

关键词： manganese oxide     bismuth vanadium tetraoxide     photocatalytic ozonation     hydroxyl radical     co-catalyst    

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Insight into the promotion mechanism of activated carbon on the monolithic honeycomb red mud catalyst

《环境科学与工程前沿（英文）》 2021年 第15卷 第5期 doi: 10.1007/s11783-020-1337-7

摘要：

• Activated carbon was proposed to be an efficient accelerant for molded red mud catalyst.

关键词： NOx     Selective catalytic reduction     Iron-based catalyst     Red mud     Monolithic catalyst     Activated carbon    

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Direct synthesis of diphenyl carbonate over heterogeneous catalyst: effects of structure of substitutedperovskite carrier on the catalyst activities

WU Guangwen, JIN Fang, WU Yuxin, ZHANG Guangxu, LI Dinghuo, WANG Cunwen, MA Peisheng

《化学科学与工程前沿（英文）》 2007年 第1卷 第1期   页码 59-64 doi: 10.1007/s11705-007-0012-x

摘要： The perovskite-type compound LaMnO was substituted for the part of La in position A and for the part of Mn in position B by citrate method. The phases were detected by X-ray diffraction. Powder morphologies were scanned by scanning electron microscopy. The valence of atoms was determined by X-ray photoelectron spectroscopy. It was found that the perovskite can form crystal defect and increase the proportion of high valence B element by doping. Active component Pd was loaded on various perovskite supports for synthesis of diphenyl carbonate. The results showed that the activities of catalysts in which supports have crystal defect by substitution were higher. It can be concluded that perovskite with defect structure by doping could lead to the formation of oxygen vacancy where the lattice oxygen became exchangeable with the oxygen gas. Also, this improved the redox process of the carrier by transferring electrons and activities of catalysts.

关键词： photoelectron spectroscopy     diphenyl carbonate     proportion     diffraction     perovskite    

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用于提高叔胺的二氧化碳吸收能力的纳米多孔碳材料促进剂的制备 Review

Masood S. Alivand, Omid Mazaheri, Yue Wu, Geoffrey W. Stevens, Colin A. Scholes, Kathryn A. Mumford

《工程（英文）》 2020年 第6卷 第12期   页码 1381-1394 doi: 10.1016/j.eng.2020.05.004

摘要：

叔胺水溶液具有吸收力强、反应热低、腐蚀性低等特点，作为一种二氧化碳（CO2）吸收剂，其应用前景良好。然而，由于叔胺吸收CO2的速率过慢，不适用于大规模实际应用。本文对一些不同特性的纳米多孔碳材料促进剂（NCP）进行了合成和表征，并将其作为N,N-二乙基乙醇胺（DEEA）水溶液吸收CO2的加速剂。通过采用超声技术将NCP注入到3 mol·L–1的DEEA水溶液中，制备得 到了DEEA-NCP纳米流体。结果表明，在与乙二胺（EDA）、聚乙烯亚胺（PEI）发生官能化反应的微孔（GC）碳材料和介孔（GS）碳材料结构中，GC-EDA促进剂的性能最佳。对比DEEAGC-EDA纳米流体与典型的DEEA水溶液得出，GC-EDA促进剂在40℃时的CO2吸收率为36.8~50.7 kPa·min–1，提高了38.6%，平衡CO2吸收率为每摩尔DEEA中CO2的含量为0.69~0.78 mol（15 kPa; 40 ℃），提高了13.2%。此外，本文测定了DEEA-GC-EDA纳米流体的可再利用性，同时还提出了循环利用的方法。本文得出结论：在叔胺中加入NCP-GC-EDA促进剂可以提高CO2吸收率，同时还有利于实现叔胺的大规模使用，其前景广阔。 

关键词： 二氧化碳吸收     纳米流体     N     N-二乙基乙醇胺     纳米多孔碳促进剂     聚胺功能化    

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Pd nano-catalyst supported on biowaste-derived porous nanofibrous carbon microspheres for efficient catalysis

《化学科学与工程前沿（英文）》 2023年 第17卷 第9期   页码 1289-1300 doi: 10.1007/s11705-023-2299-7

摘要： Environmental pollution caused by the presence of aromatic aldehydes and dyes in wastewater is a serious global concern. An effective strategy for the removal of these pollutants is their catalytic conversion, possibly to valuable compounds. Therefore, the design of efficient, stable and long-lifetime catalysts is a worthwhile research goal. Herein, we used nanofibrous carbon microspheres (NCM) derived from the carbohydrate chitin present in seafood waste, and characterized by interconnected nanofibrous networks and N/O-containing groups, as carriers for the manufacture of a highly dispersed, efficient and stable Pd nano-catalyst (mean diameter ca. 2.52 nm). Importantly, the carbonised chitin’s graphitized structure, defect presence and large surface area could promote the transport of electrons between NCM and Pd, thereby endowing NCM supported Pd catalyst with high catalytic activity. The NCM supported Pd catalyst was employed in the degradation of some representative dyes and the chemoselective hydrogenation of aromatic aldehydes; this species exhibited excellent catalytic activity and stability, as well as applicability to a broad range of aromatic aldehydes, suggesting its potential use in green industrial catalysis.

关键词： biowaste chitin     nanofibrous     palladium     nano-catalyst     catalysis    

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Advanced materials: adsorbent and catalyst for environmental application

Junhua LI, Shubo DENG

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 301-301 doi: 10.1007/s11783-013-0529-9

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标题 作者 时间 类型 操作

The catalytic effect of both oxygen-bearing functional group and ash in carbonaceous catalyst on CH 4

Weidong ZHANG, Yongfa ZHANG,

期刊论文

Effect of carbon deposition over carbonaceous catalysts on CH

Yongfa ZHANG, Meng ZHANG, Guojie ZHANG, Huirong ZHANG

期刊论文

Synthesis of magnetic carbonaceous acid derived from waste garlic peel for biodiesel production via esterification

Hewei YU, Jinke WU, Wei WEI, Xingyu ZHANG, Changzai REN, Yaoqi DONG, Shen CHENG

期刊论文

Reactivity of Pyrogenic Carbonaceous Matter (PCM) in mediating environmental reactions: Current knowledge

Wenqing Xu, Mark L. Segall, Zhao Li

期刊论文

Emission factors of gaseous carbonaceous species from residential combustion of coal and crop residue

Qin WANG, Chunmei GENG, Sihua LU, Wentai CHEN, Min SHAO

期刊论文

Interaction of carbonaceous nanomaterials with wastewater biomass

Yu YANG,Zhicheng YU,Takayuki NOSAKA,Kyle DOUDRICK,Kiril HRISTOVSKI,Pierre HERCKES,Paul WESTERHOFF

期刊论文

Modeling nanostructured catalyst layer in PEMFC and catalyst utilization

Jiejing ZHANG, Pengzhen CAO, Li XU, Yuxin WANG

期刊论文

Oxidant or catalyst for oxidation?

Jianzhi Huang, Huichun Zhang

期刊论文

Monte Carlo simulation of the PEMFC catalyst layer

WANG Hongxing, CAO Pengzhen, WANG Yuxin

期刊论文

Dendritic BiVO4 decorated with MnOx co-catalyst as an efficient hierarchical catalyst for photocatalytic

Jin Yang, Xuelian Liu, Hongbin Cao, Yanchun Shi, Yongbing Xie, Jiadong Xiao

期刊论文

Insight into the promotion mechanism of activated carbon on the monolithic honeycomb red mud catalyst

期刊论文

Direct synthesis of diphenyl carbonate over heterogeneous catalyst: effects of structure of substitutedperovskite carrier on the catalyst activities

WU Guangwen, JIN Fang, WU Yuxin, ZHANG Guangxu, LI Dinghuo, WANG Cunwen, MA Peisheng

期刊论文

用于提高叔胺的二氧化碳吸收能力的纳米多孔碳材料促进剂的制备

Masood S. Alivand, Omid Mazaheri, Yue Wu, Geoffrey W. Stevens, Colin A. Scholes, Kathryn A. Mumford

期刊论文

Pd nano-catalyst supported on biowaste-derived porous nanofibrous carbon microspheres for efficient catalysis

期刊论文

Advanced materials: adsorbent and catalyst for environmental application

Junhua LI, Shubo DENG

期刊论文