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Amino acid promoted hydrogen battery system using Mn-pincer complex for reversible CO hydrogenation toformic acid

《能源前沿（英文）》 2022年 第16卷 第5期   页码 697-699 doi: 10.1007/s11708-022-0843-7

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A Pt-Bi bimetallic nanoparticle catalyst for direct electro-oxidation of formic acid in fuel cells

Shu-Hong LI, Yue ZHAO, Jian CHU, Wen-Wei LI, Han-Qing YU, Gang LIU, Yang-Chao TIAN

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 388-394 doi: 10.1007/s11783-012-0475-y

摘要： Direct formic acid fuel cells are a promising portable power-generating device, and the development of efficient anodic catalysts is essential for such a fuel cell. In this work Pt-Bi nanoparticles supported on micro-fabricated gold wire array substrate were synthesized using an electrochemical deposition method for formic acid oxidation in fuel cells. The surface morphology and element components of the Pt-Bi/Au nanoparticles were characterized, and the catalytic activities of the three Pt-Bi/Au nanoparticle electrodes with different Pt/Bi ratios for formic acid oxidation were evaluated. It was found that Pt Bi /Au had a much higher catalytic activity than Pt Bi /Au and Pt Bi /Au, and Pt Bi /Au exhibited a current density of 2.7 mA·cm , which was 27-times greater than that of Pt/Au. The electro-catalytic activity of the Pt-Bi/Au electrode for formic acid oxidation increased with the increasing Bi content, suggesting that it would be possible to achieve an efficient formic acid oxidation on the low Pt-loading. Therefore, the Pt-Bi/Au electrode offers a promising catalyst with a high activity for direct oxidation of formic acid in fuel cells.

关键词： catalyst     electrochemical deposition     formic acid oxidation     fuel cell     gold wire array     microfabrication    

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degradation of carbon tetrachloride by carbon dioxide radical anion-based sodium percarbonate/ Fe(II)/formicacid system in aqueous solution

Wenchao Jiang, Ping Tang, Shuguang Lu, Xiang Zhang, Zhaofu Qiu, Qian Sui

《环境科学与工程前沿（英文）》 2018年 第12卷 第2期 doi: 10.1007/s11783-017-0987-6

摘要： The performance of sodium percarbonate (SPC) activated with ferrous ion (Fe(II)) with the addition of formic acid (FA) to stimulate the degradation of carbon tetrachloride (CT) was investigated. Results showed that CT could be entirely reduced within 15 min in the system at a variety of SPC/Fe(II)/FA/CT molar ratios in experimental level. Scavenging tests indicated that carbon dioxide radical anion (CO2· ) was the dominant reactive oxygen species responsible for CT degradation. CT degradation rate, to a large extent, increased with increasing dosages of chemical agents and the optimal molar ratio of SPC/Fe(II)/FA/CT was set as 60/60/60/1. The initial concentration of CT can hardly affect the CT removal, while CT degradation was favorable in the pH range of 3.0–9.0, but apparently inhibited at pH 12. Cl and HCO of high concentration showed negative impact on CT removal. Cl released from CT was detected and the results confirmed nearly complete mineralization of CT. CT degradation was proposed by reductive C-Cl bond splitting. This study demonstrated that SPC activated with Fe(II) with the addition of FA may be promising technique for CT remediation in contaminated groundwater.

关键词： Carbon tetrachloride     Sodium percarbonate     Formic acid     Reductive radicals     Groundwater    

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Nitrogen-doped carbon black supported Pd nanoparticles as an effective catalyst for formic acid electro-oxidation

Na SUN, Minglei WANG, Jinfa CHANG, Junjie GE, Wei XING, Guangjie SHAO

《能源前沿（英文）》 2017年 第11卷 第3期   页码 310-317 doi: 10.1007/s11708-017-0491-5

摘要： Pd nanoparticles supported on nitrogen doped carbon black (Vulcan XC-72R) with two different levels of doping were prepared by the microwave-assisted ethylene glycol reduction process and used as catalyst for the formic acid electro-oxidation (FAEO). The results indicate that the different nitrogen doping contents in Pd/N-C catalysts have a significant effect on the performance of FAEO. A higher N content facilitates the uniform dispersion of Pd nanoparticles on carbon black with narrow particle size distribution. Furthermore, the electrochemical results show that the catalyst with a higher N-doping content possesses a higher catalytic activity and a long-term stability for FAEO. The peak current density of the Pd/N-C (high) catalyst is 1.27 and 2.31 times that of the Pd/N-C (low) and homemade Pd/C-H catalyst. The present paper may provide a simple method for preparation of high-performance anode catalyst for direct formic acid fuel cells (DFAFCs).

关键词： formic acid electro-oxidation     nitrogen doped     oxidized carbon     nitrogen content    

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Degradation of carbon tetrachloride in thermally activated persulfate system in the presence of formicacid

Minhui XU,Xiaogang GU,Shuguang LU,Zhouwei MIAO,Xueke ZANG,Xiaoliang WU,Zhaofu QIU,Qian SUI

《环境科学与工程前沿（英文）》 2016年 第10卷 第3期   页码 438-446 doi: 10.1007/s11783-015-0798-6

摘要： The thermally activated persulfate (PS) degradation of carbon tetrachloride (CT) in the presence of formic acid (FA) was investigated. The results indicated that CT degradation followed a zero order kinetic model, and was responsible for the degradation of CT confirmed by radical scavenger tests. CT degradation rate increased with increasing PS or FA dosage, and the initial CT had no effect on CT degradation rate. However, the initial solution pH had effect on the degradation of CT, and the best CT degradation occurred at initial pH 6. Cl had a negative effect on CT degradation, and high concentration of Cl displayed much strong inhibition. Ten mmol·L promoted CT degradation, while 100 mmol·L inhibited the degradation of CT, but promoted CT degradation in the presence of FA. The measured Cl concentration released into solution along with CT degradation was 75.8% of the total theoretical dechlorination yield, but no chlorinated intermediates were detected. The split of C-Cl was proposed as the possible reaction pathways in CT degradation. In conclusion, this study strongly demonstrated that the thermally activated PS system in the presence of FA is a promising technique in in situ chemical oxidation (ISCO) remediation for CT contaminated site.

关键词： persulfate     carbon tetrachloride     thermal activation     formic acid     carbon dioxide radical anion    

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Formic acid dehydrogenation reaction on high-performance PdAu alloy nanoparticles prepared by the eco-friendly

《能源前沿（英文）》   页码 751-762 doi: 10.1007/s11708-023-0895-3

摘要： Dehydrogenation of formic acid (FA) is considered to be an effective solution for efficient storage and transport of hydrogen. For decades, highly effective catalysts for this purpose have been widely investigated, but numerous challenges remain. Herein, the PdxAu1−x (x = 0, 0.2, 0.4, 0.5, 0.6, 0.8, 1) alloys over the whole composition range were successfully prepared and used to catalyze FA hydrogen production efficiently near room temperature. Small PdAu nanoparticles (5–10 nm) were well-dispersed and supported on the activated carbon to form PdAu solid solution alloys via the eco-friendly slow synthesis methodology. The physicochemical properties of the PdAu alloys were comprehensively studied by utilizing various measurement methods, such as X-ray diffraction (XRD), N2 adsorption–desorption, high angle annular dark field-scanning transmission electron microscope (HAADF-STEM), X-ray photoelectrons spectroscopy (XPS). Notably, owing to the strong metal-support interaction (SMSI) and electron transfer between active metal Au and Pd, the Pd0.5Au0.5 obtained exhibits a turnover frequency (TOF) value of up to 1648 h−1 (313 K, nPd+Au/nFA = 0.01, nHCOOH/nHCOONa = 1:3) with a high activity, selectivity, and reusability in the FA dehydrogenation.

关键词： FA dehydrogenation     face-centred cubic structures     PdAu solid solution alloy nanoparticles     slow synthesis methodology     SMSI effect    

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Electrodeposited porous Pb electrode with improved electrocatalytic performance for the electroreduction of CO

Jing WANG, Hua WANG, Zhenzhen HAN, Jinyu HAN

《化学科学与工程前沿（英文）》 2015年 第9卷 第1期   页码 57-63 doi: 10.1007/s11705-014-1444-8

摘要： A porous Pb foam was fabricated electrochemically at a copper substrate and then used as the cathode for the electroreduction of CO . The surface morphology and composition of the porous Pb electrode was characterized by scanning electron microscopy, X-ray diffraction, transmission electron microscopy and selected area electron diffraction. The honeycomb-like porous structure was composed of needle-like Pb deposits. Cyclic voltammetry studies demonstrated that the porous Pb electrode had better electrocatalytic performance for the formation of formic acid from CO compared with a Pb plate electrode. The increase in current density was due to the large surface area of the porous Pb electrode, which provides more active sites on the electrode surface. The improved formic acid selectivity was due to the morphology of the roughened surface, which contains significantly more low-coordination sites which are more active for CO reduction. The highest current efficiency for formic acid was 96.8% at -1.7 V versus saturated calomel electrode at 5 °C. This porous Pb electrode with good catalytic abilities represents a new 3D porous material with applications for the electroreduction of CO .

关键词： electrodeposited porous Pb     carbon dioxide     electroreduction     formic acid    

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Preparation of a Pb loaded gas diffusion electrode and its application to CO

Ang LI, Hua WANG, Jinyu HAN, Li LIU

《化学科学与工程前沿（英文）》 2012年 第6卷 第4期   页码 381-388 doi: 10.1007/s11705-012-1216-2

摘要： A Pb loaded gas diffusion electrode was fabricated and used for the electroreduction of CO to formic acid. The Pb/C catalyst was prepared by isometric impregnation. The crystal structure and morphology of the Pb/C catalyst were characterized by X-ray diffraction (XRD) and transmission electron microscope (TEM). The preparation conditions of the gas diffusion electrode were optimized by adjusting the amounts of polytetrafluoroethylene (PTFE) in the gas diffusion layer and acetylene black in the catalytic layer. The electrochemical performance of the as-prepared gas diffusion electrode was studied by chronoamperometry and cyclic voltammetry. The optimized gas diffusion electrode showed good catalytic performance for the electroreduction of CO . The current efficiency of formic acid after 1 h of operation reached a maximum of 22% at -2.0 V versus saturated calomel electrode (SCE).

关键词： electroreduction     carbon dioxide     lead catalyst     gas diffusion electrode     formic acid    

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tetrachloride degradation by hydroxylamine in ferrous ion activated calcium peroxide in the presence of formicacid

Wenchao Jiang, Ping Tang, Zhen Liu, Huan He, Qian Sui, Shuguang Lyu

《环境科学与工程前沿（英文）》 2020年 第14卷 第2期 doi: 10.1007/s11783-019-1197-1

摘要： Complete CT degradation was achieved by employing HA to CP/Fe(II)/FA process. Quantitative detection of Fe(II) regeneration and HO• production was investigated. Benzoic acid outcompeted FA for the reaction with HO•. CO2•− was the dominant reductive radical for CT removal. Effects of solution matrix on CT removal were conducted. Hydroxyl radicals (HO•) show low reactivity with perchlorinated hydrocarbons, such as carbon tetrachloride (CT), in conventional Fenton reactions, therefore, the generation of reductive radicals has attracted increasing attention. This study investigated the enhancement of CT degradation by the synergistic effects of hydroxylamine (HA) and formic acid (FA) (initial [CT] = 0.13 mmol/L) in a Fe(II) activated calcium peroxide (CP) Fenton process. CT degradation increased from 56.6% to 99.9% with the addition of 0.78 mmol/L HA to the CP/Fe(II)/FA/CT process in a molar ratio of 12/6/12/1. The results also showed that the presence of HA enhanced the regeneration of Fe(II) from Fe(III), and the production of HO• increased one-fold when employing benzoic acid as the HO• probe. Additionally, FA slightly improves the production of HO•. A study of the mechanism confirmed that the carbon dioxide radical (CO2•−), a strong reductant generated by the reaction between FA and HO•, was the dominant radical responsible for CT degradation. Almost complete CT dechlorination was achieved in the process. The presence of humic acid and chloride ion slightly decreased CT removal, while high doses of bicarbonate and high pH inhibited CT degradation. This study helps us to better understand the synergistic roles of FA and HA for HO• and CO2•− generation and the removal of perchlorinated hydrocarbons in modified Fenton systems.

关键词： Calcium peroxide     Hydroxylamine     Modified Fenton     Reactive oxygen species     Perchlorinated hydrocarbon    

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Sulfonic acid-functionalized mesoporous silica catalyst with different morphology for biodiesel production

《化学科学与工程前沿（英文）》 2022年 第16卷 第8期   页码 1198-1210 doi: 10.1007/s11705-021-2133-z

摘要： Sulfonic acid functionalized mesoporous silica based solid acid catalysts with different morphology were designed and fabricated. The synthesized materials were characterized by various physicochemical and spectroscopic techniques like scanning electron microscope-energy dispersive X-ray spectroscopy, Fourier transform infrared spectroscopy, Brunauer–Emmett–Teller surface area, thermogravimetric analysis and n-butylamine acidity. The shape of catalysts particles plays an important role in its activity. The sulfonic acid functionalized mesoporous silica catalysts of spherical shape and the cube shape were assessed for catalytic activity in biodiesel production. The catalytic biodiesel production reaction over the catalysts were studied by esterification of free fatty acid, oleic acid with methanol. The effect of various reaction parameters such as catalyst concentration, acid/alcohol molar ratio, catalyst amount, reaction temperature and reaction time on catalytic activity were investigated to optimize the conditions for maximum conversion. It was sulfonated cubic shape mesoporous silica which exhibited better activity as compared to the spherical shape silica catalysts. Additionally, the catalyst was regenerated and reused up to three cycles without any significant loss in activity. The present catalysts exhibit superior performance in biodiesel production and it can be used for the several biodiesel feedstock’s that are rich in free fatty acids.

关键词： solid acid catalyst     mesoporous silica     sulfonic acid     biodiesel     esterification     oleic acid    

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Enzyme@bismuth-ellagic acid: a versatile platform for enzyme immobilization with enhanced acid-base stability

《化学科学与工程前沿（英文）》 2023年 第17卷 第6期   页码 784-794 doi: 10.1007/s11705-022-2278-4

摘要： In situ encapsulation is an effective way to synthesize enzyme@metal–organic framework biocatalysts; however, it is limited by the conditions of metal–organic framework synthesis and its acid-base stability. Herein, a biocatalytic platform with improved acid-base stability was constructed via a one-pot method using bismuth-ellagic acid as the carrier. Bismuth-ellagic acid is a green phenol-based metal–organic framework whose organic precursor is extracted from natural plants. After encapsulation, the stability, especially the acid-base stability, of amyloglucosidases@bismuth-ellagic acid was enhanced, which remained stable over a wide pH range (2–12) and achieved multiple recycling. By selecting a suitable buffer, bismuth-ellagic acid can encapsulate different types of enzymes and enable interactions between the encapsulated enzymes and cofactors, as well as between multiple enzymes. The green precursor, simple and convenient preparation process provided a versatile strategy for enzymes encapsulation.

关键词： bismuth-ellagic acid     in situ encapsulation     enzyme@MOF biocomposites    

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Discovery of novel ursolic acid derivatives as effective antimicrobial agents through a ROS-mediated

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 2101-2113 doi: 10.1007/s11705-023-2361-5

摘要： In response to the reduction of food production and economic losses caused by plant bacterial diseases, it is necessary to develop new, efficient, and green pesticides. Natural products are rich and sustainable source for the development of new pesticides due to their low toxicity, easy degradation, and eco-friendliness. In this study, we prepared three series of ursolic acid derivatives and assessed their antibacterial ability. Most target compounds exhibited outstanding antibacterial activities. Among them, the relative optimal EC50 values of Xanthomonas oryzae pv. oryzae and Xanthomonas axonopodis pv. citri were 2.23 (A17) and 1.39 (A16) μg·mL–1, respectively. The antimicrobial mechanism showed that compound A17 induced an excessive accumulation and production of reactive oxygen species in bacteria and damaged the cell membrane integrity to kill bacteria. More interestingly, the addition of low concentrations of exogenous hydrogen peroxide enhanced the antibacterial efficacy of compound A17 against Xanthomonas oryzae pv. oryzae. These entertaining results suggested that compound A17 induced an apparent apoptotic behavior in the tested bacteria. Overall, we developed the promising antimicrobial agents that destroyed the redox system of phytopathogenic bacteria, further demonstrating the unprecedented potential of ursolic acid for agricultural applications.

关键词： ursolic acid     antibacterial activities     reactive oxygen species     apoptosis    

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Synergistic scale inhibition of polyaspartic acid composite with magnetic field

LIU Zhenfa, WANG Yanji, GAO Yuhua, ZHANG Lihui

《化学科学与工程前沿（英文）》 2007年 第1卷 第3期   页码 261-265 doi: 10.1007/s11705-007-0047-z

摘要： Polyaspartic acid (PASP) composite, a scale inhibitor, was prepared from PASP, itaconic acid–acrylic acid–acrylic ester (IA-AA-AE) terpolymer and 2-phosphonobutane- 1,2,4-tricarboxylic acid (PBTCA). The scale inhibition of PASP composite and the effect of its synergism with a magnetic field on scale inhibition were investigated. Calcium carbonate crystals in scale samples were characterized by means of SEM and XRD. The static and dynamic experiments show that the chelating function of PASP composite for Ca can be enhanced by synergism with a magnetic field. Under Ca 650 mg/L, HCO 1,300 mg/L and PASP composite 4 mg/L, the scale inhibition rate of PASP composite in magnetic water can increase by 10% in static state and by 20% in dynamic experiments. Scanning electron microscope (SEM) and X-ray diffraction (XRD) results show that calcite and aragonite can be completely transformed into vaterite by using PASP composite.

关键词： synergism     magnetic     PBTCA     dynamic     acid–acrylic acid–acrylic    

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Abiotic association of phthalic acid esters with humic acid of a sludge landfill

Xiaoli CHAI, Yongxia HAO, Xin ZHAO, Guixiang LIU, Ying ZHU, Rong JI, Jun WU, Huanhuan TONG, Youcai ZHAO

《环境科学与工程前沿（英文）》 2012年 第6卷 第6期   页码 778-783 doi: 10.1007/s11783-012-0434-7

摘要： The abiotic association between phthalic acid esters (PAEs) and humic substances (HS) in sludge landfill plays an important role in the fate and stability of PAEs. An equilibrium dialysis combined with C-labeling was used to study the abiotic association of two abundant PAEs (diethyl phthalate and di- -butyl phthalate) with humic acid (HA) isolated from a sludge landfill with different stabilization times and different molecular weights. Elemental analysis and Fourier Transform Infrared Spectrophotometer (FTIR) suggested that high value of HA was related to the high aromatic content and large molecular weight of HA. The results indicated that the association strength of PAEs with HA depended on both the properties of the PAEs and the characteristics of HA. The values of the association were strongly dependent on solution pH, and decreased dramatically as the pH was increased from 3.0 to 9.0. The results suggested that non-specific hydrophobic interaction between PAEs and HA was the main contributor to the association of the PAEs with HA. The interactive hydrogen-bonds between the HA and the PAEs molecules may also be involved in the association.

关键词： abiotic association     phthalic acid esters (PAEs)     humic acid     sludge     landfill    

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New perspectives in free nitrous acid (FNA) uses for sustainable wastewater management

《环境科学与工程前沿（英文）》 2023年 第18卷 第2期 doi: 10.1007/s11783-024-1786-5

摘要：

● The historical development of free nitrous acid (FNA) technologies is reviewed.

关键词： Free nitrous acid     Acid-tolerant ammonia oxidizer     In situ generation     Wastewater management    

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标题 作者 时间 类型 操作

Amino acid promoted hydrogen battery system using Mn-pincer complex for reversible CO hydrogenation toformic acid

期刊论文

A Pt-Bi bimetallic nanoparticle catalyst for direct electro-oxidation of formic acid in fuel cells

Shu-Hong LI, Yue ZHAO, Jian CHU, Wen-Wei LI, Han-Qing YU, Gang LIU, Yang-Chao TIAN

期刊论文

degradation of carbon tetrachloride by carbon dioxide radical anion-based sodium percarbonate/ Fe(II)/formicacid system in aqueous solution

Wenchao Jiang, Ping Tang, Shuguang Lu, Xiang Zhang, Zhaofu Qiu, Qian Sui

期刊论文

Nitrogen-doped carbon black supported Pd nanoparticles as an effective catalyst for formic acid electro-oxidation

Na SUN, Minglei WANG, Jinfa CHANG, Junjie GE, Wei XING, Guangjie SHAO

期刊论文

Degradation of carbon tetrachloride in thermally activated persulfate system in the presence of formicacid

Minhui XU,Xiaogang GU,Shuguang LU,Zhouwei MIAO,Xueke ZANG,Xiaoliang WU,Zhaofu QIU,Qian SUI

期刊论文

Formic acid dehydrogenation reaction on high-performance PdAu alloy nanoparticles prepared by the eco-friendly

期刊论文

Electrodeposited porous Pb electrode with improved electrocatalytic performance for the electroreduction of CO

Jing WANG, Hua WANG, Zhenzhen HAN, Jinyu HAN

期刊论文

Preparation of a Pb loaded gas diffusion electrode and its application to CO

Ang LI, Hua WANG, Jinyu HAN, Li LIU

期刊论文

tetrachloride degradation by hydroxylamine in ferrous ion activated calcium peroxide in the presence of formicacid

Wenchao Jiang, Ping Tang, Zhen Liu, Huan He, Qian Sui, Shuguang Lyu

期刊论文

Sulfonic acid-functionalized mesoporous silica catalyst with different morphology for biodiesel production

期刊论文

Enzyme@bismuth-ellagic acid: a versatile platform for enzyme immobilization with enhanced acid-base stability

期刊论文

Discovery of novel ursolic acid derivatives as effective antimicrobial agents through a ROS-mediated

期刊论文

Synergistic scale inhibition of polyaspartic acid composite with magnetic field

LIU Zhenfa, WANG Yanji, GAO Yuhua, ZHANG Lihui

期刊论文

Abiotic association of phthalic acid esters with humic acid of a sludge landfill

Xiaoli CHAI, Yongxia HAO, Xin ZHAO, Guixiang LIU, Ying ZHU, Rong JI, Jun WU, Huanhuan TONG, Youcai ZHAO

期刊论文

New perspectives in free nitrous acid (FNA) uses for sustainable wastewater management

期刊论文