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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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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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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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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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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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Electrochemical oxidation of humic acid at the antimony- and nickel-doped tin oxide electrode

TANG Chengli,YAN Wei,ZHENG Chunli

《环境科学与工程前沿（英文）》 2014年 第8卷 第3期   页码 337-344 doi: 10.1007/s11783-013-0545-9

摘要： This work investigated the degradation of humic acid (HA) in aqueous solution by electrochemical oxidation with Antimony- and Nickel-doped Tin oxide electrode (Ni-Sb-SnO /Ti electrode) as the anode. Initial concentrations of HA ranged from 3 to 9 mg·L . Under such a concentration scope, the degradation of HA was a mass transfer controlled process. Degradation rate increased with the increase of HA initial concentration. Test on the effect of tert-butanol revealed that ·OH played an important role in the oxidation of HA. The absence of cation Ca was beneficial to HA degradation, which suggested that both indirect and direct electrolyze happened during the whole electrochemical oxidation process. Alkaly (pH= 12) and neutral (pH= 7) conditions were benefical to HA degradation.

关键词： electrochemical oxidation     humic acid (HA)     natural water     Ni-Sb-SnO2/Ti electrode    

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Anodic oxidation of azo dye C.I. Acid Red 73 by the yttrium-doped Ti/SnO

Li XU, Zhi GUO, Lishun DU

《化学科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 338-346 doi: 10.1007/s11705-013-1335-4

摘要： This work was conducted to study the ability of anodic oxidation of azo dye C.I. Acid Red 73 (AR73) using the yttrium-doped Ti/SnO -Sb electrodes. The effects of Sb doping level, yttrium doping level, thermal decomposition temperature and cycle times of dip-coating thermal decomposition on the properties of the electrodes were investigated. The results showed that the excellent electrochemical activity of Ti/SnO -Sb-Y electrode can be achieved at a 7∶1 molar ratio of Sn∶Sb and thermal decomposition temperature of 550°C. Moreover when the cycle times of dip-coating and thermal decomposition were up to 10 times, the performance of the electrode tends to be stable. The Ti/SnO -Sb electrodes doped with yttrium (0.5 mol-%) showed the most excellent electrochemical activity. In addition, the influences of operating variables, including current density, initial pH, dye concentration and support electrolyte, on the colour removal, chemical oxygen demand (COD) removal and current efficiency were also investigated. Our results confirmed that the current efficiency increased with the concentrations of dye and sodium chloride. Moreover, increasing the current density and the initial pH would reduce the current efficiency.

关键词： SnO2-Sb     yttrium doping     anodic oxidation     azo dyes    

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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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Identification and ecotoxicity assessment of intermediates generated during the degradation of clofibric acidby advanced oxidation processes

Wenzhen LI, Yu DING, Qian SUI, Shuguang LU, Zhaofu QIU, Kuangfei LIN

《环境科学与工程前沿（英文）》 2012年 第6卷 第4期   页码 445-454 doi: 10.1007/s11783-012-0419-6

摘要： The aim of this study was to identify the intermediates in clofibric acid degradation under various advanced oxidation processes, namely ultraviolet (UV), UV/H O , vacuum ultraviolet (VUV), VUV/H O , and solar/TiO processes, as well as to assess the toxicity of these intermediates. Eleven intermediates have been detected by gas chromatography-mass spectrometer, most of which were reported for the first time to our best knowledge. Combining the evolution of the dissolved organic carbon, Cl and specific ultraviolet absorption at 254 nm, it could be deduced that cleavage of aromatic ring followed by dechlorination was the mechanism in solar/TiO process, while dechlorination happened first and accumulation of aromatic intermediates occurred in the other processes. Different transformation pathways were proposed for UV-, VUV-assisted and solar/TiO processes, respectively. The acute toxicity was evaluated by means of T spp. bioassay. It was believed that aromatic intermediates increased the toxicity and the ring-opening pathway in solar/TiO process could relieve the toxicity.

关键词： clofibric acid     advanced oxidation processes     intermediates     toxicity     Photobacterium phosphoreum T3 spp.    

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Plasma-assisted oxidation of benzoic acid

Anna Khlyustova, Nikolay Sirotkin

《化学科学与工程前沿（英文）》 2020年 第14卷 第4期   页码 513-521 doi: 10.1007/s11705-019-1825-0

摘要： Plasma-assisted oxidation of organic compounds is one of the developing technologies for wastewater treatment. Plasmas effectively accelerate degradation processes due to plasma generated reactive species and ultra-violet radiation. Oxidation of benzoic acid in aqueous solutions by the atmospheric pressure glow discharge and underwater diaphragm discharge was studied and monitored by fluorescence and spectrophotometric methods. Discharge type and solution pH affect the formation rates of mono- and dihydroxybenzoic acids. Dihydroxyl derivatives were formed only by glow discharge action. The yields of hydroxyl radical were estimated on the kinetics data for the hydroxylation of benzoic acid. The steps of the hydroxylation processes and further oxidation were described.

关键词： atmospheric pressure glow discharge     underwater diaphragm discharge     oxidation     benzoic acid     hydroxyl radical    

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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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Efficient base-free oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid over copper-doped

Feng Cheng, Dongwen Guo, Jinhua Lai, Meihui Long, Wenguang Zhao, Xianxiang Liu, Dulin Yin

《化学科学与工程前沿（英文）》 2021年 第15卷 第4期   页码 960-968 doi: 10.1007/s11705-020-1999-5

摘要： 2,5-Furandicarboxylic acid (FDCA) is an important and renewable building block and can serve as an alternative to terephthalic acid in the production of bio-based degradable plastic. In this study, Cu-doped MnO  nanorods were prepared by a facile hydrothermal redox method and employed as catalysts for the selective oxidation of 5-hydroxymethylfurfural (HMF) to FDCA using -butyl hydroperoxide (TBHP) as an oxidant. The catalysts were characterized using X-ray diffraction analysis, Fourier transform infrared spectroscopy, thermogravimetric analysis, and transmission electron microscopy. The effects of oxidants, solvents, and reaction conditions on the oxidation of HMF were investigated, and a reaction mechanism was proposed. Experimental results demonstrated that 99.4% conversion of HMF and 96.3% selectivity of FDCA were obtained under suitable conditions, and -butanol was the most suitable solvent when TBHP was used as an oxidant. More importantly, the Cu-doped MnO catalyst can maintain durable catalytic activity after being recycled for more than ten times.

关键词： 5-hydroxymethylfurfural     25-furandicarboxylic acid     selective oxidation     Cu-doped MnO2     biomass transformation    

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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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Acid Orange 7 degradation using methane as the sole carbon source and electron donor

《环境科学与工程前沿（英文）》 2022年 第16卷 第3期 doi: 10.1007/s11783-021-1468-5

摘要：

• AO7 degradation was coupled with anaerobic methane oxidation.

关键词： Azo dyes     AO7 degradation     Anaerobic methane oxidation     Microbial community     ANME-2d    

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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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标题 作者 时间 类型 操作

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

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

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

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

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

Electrochemical oxidation of humic acid at the antimony- and nickel-doped tin oxide electrode

TANG Chengli,YAN Wei,ZHENG Chunli

期刊论文

Anodic oxidation of azo dye C.I. Acid Red 73 by the yttrium-doped Ti/SnO

Li XU, Zhi GUO, Lishun DU

期刊论文

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

期刊论文

Identification and ecotoxicity assessment of intermediates generated during the degradation of clofibric acidby advanced oxidation processes

Wenzhen LI, Yu DING, Qian SUI, Shuguang LU, Zhaofu QIU, Kuangfei LIN

期刊论文

Plasma-assisted oxidation of benzoic acid

Anna Khlyustova, Nikolay Sirotkin

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

Efficient base-free oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid over copper-doped

Feng Cheng, Dongwen Guo, Jinhua Lai, Meihui Long, Wenguang Zhao, Xianxiang Liu, Dulin Yin

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

Acid Orange 7 degradation using methane as the sole carbon source and electron donor

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