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Efficient dechlorination of 2,4-dichlorophenol in an aqueous media with a mild pH using a Pd/TiO

Jiangkun DU,Jianguo BAO,Wei HU

《环境科学与工程前沿（英文）》 2015年 第9卷 第5期   页码 919-928 doi: 10.1007/s11783-015-0794-x

摘要： In this study, palladium-loaded titania nanotubes was fabricated on a titanium plate (Pd/TiO NTs/Ti) for efficient electrodechlorination of 2,4-chlorophenol with a mild pH condition. The nature of Pd/TiO NTs/Ti electrodes was characterized by field-emission scanning electron microscope (FESEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and cyclic voltammetry (CV) techniques. The characterization results indicated the generation of Pd nanoparticles which were evenly dispersed on titania nanotubes arrays on the Pd/TiO NTs/Ti surface. An effective degradation efficiency of up to 91% was achieved within 60 min at cathode potential of −0.7 V ( SCE) and initial pH of 5.5. The effects of the applied cathode potential and initial pH on the degradation efficiency were studied. A near neutral condition was more favorable since very low and very high pHs were not conducive to the dechlorination process. Furthermore, the intermediates analysis showed that the Pd/TiO NTs/Ti electrode could completely remove chlorine from 2, 4-dichlorophenol since only phenol was detected as the byproduct and the concentration of released chlorine ions indicated near-complete dechlorination. This work presents a good alternative technique for eliminating persistent chlorophenols in polluted wastewater without maintaining strong acidic environment.

关键词： Pd/TiO2NTs/Ti cathode     chlorophenols     electrocatalytic dechlorination     wastewater treatment    

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Competition for electrons between reductive dechlorination and denitrification

Lifeng Cao, Weihua Sun, Yuting Zhang, Shimin Feng, Jinyun Dong, Yongming Zhang, Bruce E. Rittmann

《环境科学与工程前沿（英文）》 2017年 第11卷 第6期 doi: 10.1007/s11783-017-0959-x

摘要： It is common that 2,4,6-trichlorophenol (TCP) coexists with nitrate or nitrite in industrial wastewaters. In this work, simultaneous reductive dechlorination of TCP and denitrification of nitrate or nitrite competed for electron donor, which led to their mutual inhibition. All inhibitions could be relieved to a certain degree by augmenting an organic electron donor, but the impact of the added electron donor was strongest for TCP. For simultaneous reduction of TCP together with nitrate, TCP’s removal rate value increased 75% and 150%, respectively, when added glucose was increased from 0.4 mmol·L to 0.5 mmol·L and to 0.76 mmol·L . For comparison, the removal rate for nitrate increased by only 25% and 114% for the same added glucose. The relationship between their initial biodegradation rates versus their initial concentrations could be represented well with the Monod model, which quantified their half-maximum-rate concentration ( value), and values for TCP, nitrate, and nitrite were larger with simultaneous reduction than independent reduction. The increases in are further evidence that competition for the electron donor led to mutual inhibition. For bioremediation of wastewater containing TCP and oxidized nitrogen, both reduction reactions should proceed more rapidly if the oxidized nitrogen is nitrite instead of nitrate and if readily biodegradable electron acceptor is augmented.

关键词： Competition for electrons     Denitrification     Reductive dechlorination     Bioremediation     Nitrate     2     4     6-trichlorophenol    

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Application of electrode materials and catalysts in electrocatalytic treatment of dye wastewater

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1427-1443 doi: 10.1007/s11705-021-2108-0

摘要： The dye industry produces a large amount of hazardous wastewater every day worldwide, which brings potential threaten to the global environment. As an excellent method for removal of water chroma and chemical oxygen demand, electrocatalytic methods are currently widely used in the treatment of dye wastewater. The selection and preparation of electrode materials and electrocatalysts play an important role on the electrocatalytic treatment. The aim of this paper is to introduce the most excellent high-efficiency electrode materials and electrocatalysts in the field of dye wastewater treatment. Many electrode materials such as metal electrode materials, boron-doped diamond anode materials and three-dimensional electrode are introduced in detail. Besides, the mechanism of electrocatalytic oxidation is summarized. The composite treatment of active electrode and electrocatalyst are extensively examined. Finally, the progress of photo-assisted electrocatalytic methods of dye wastewater and the catalysts are described.

关键词： electrocatalytic oxidation     electrode     electrocatalysis     dye wastewater    

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Development and characterization of an anaerobic microcosm for reductive dechlorination of PCBs

Dawei Liang, Shanquan Wang

《环境科学与工程前沿（英文）》 2017年 第11卷 第6期 doi: 10.1007/s11783-017-0939-1

摘要： The toxic and recalcitrant polychlorinated biphenyls (PCBs) adversely affect human and biota by bioaccumulation and biomagnification through food chain. In this study, an anaerobic microcosm was developed to extensively dechlorinate hexa- and hepta-CBs in Aroclor 1260. After 4 months of incubation in defined mineral salts medium amended PCBs (70 mmol·L ) and lactate (10 mmol·L ), the culture dechlorinated hexa-CBs from 40.2% to 8.7% and hepta-CBs 33.6% to 11.6%, with dechlorination efficiencies of 78.3% and 65.5%, respectively (all in moL ratio). This dechlorination process led to tetra-CBs (46.4%) as the predominant dechlorination products, followed by penta- (22.1%) and tri-CBs (5.4%). The number of chlorines per biphenyl decreased from 2.50 to 1.41. Results of quantitative real-time PCR show that cells increased from 2.39 × 10 ±0.5 × 10 to 4.99 × 10 ±0.32 × 10 copies mL after 120 days of incubation, suggesting that play a major role in reductive dechlorination of PCBs. This study could prove the feasibility of anaerobic reductive culture enrichment for the dehalogenation of highly chlorinated PCBs, which is prior to be applied for in situ bioremediation of notorious halogenated compounds.

关键词： Polychlorinated biphenyls (PCBs)     Microbial reductive dechlorination     Dehalococcoides     Pathway    

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Multivalent manganese oxides with high electrocatalytic activity for oxygen reduction reaction

Xiangfeng Peng, Zhenhai Wang, Zhao Wang, Yunxiang Pan

《化学科学与工程前沿（英文）》 2018年 第12卷 第4期   页码 790-797 doi: 10.1007/s11705-018-1706-y

摘要： A noble-metal-free catalyst based on both Mn O and MnO was prepared by using the dielectric barrier discharge technique at moderate temperature. The prepared catalyst shows a higher electrocatalytic activity towards the oxygen reduction reaction than the catalyst prepared by using the traditional calcination process. The enhanced activity could be due to the coexistence of manganese ions with different valences, the higher oxygen adsorption capacity, and the suppressed aggregation of the catalyst nanoparticles at moderate temperature. The present work would open a new way to prepare low-cost and noble-metal-free catalysts at moderate temperature for more efficient electrocatalysis.

关键词： oxygen reduction reaction     manganese oxides     mixed valences of manganese     oxygen adsorption     dielectric barrier discharge    

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Electrodeposited porous Pb electrode with improved electrocatalytic performance for the electroreduction

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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Noble-metal-free cobalt hydroxide nanosheets for efficient electrocatalytic oxidation

Jie Lan, Daizong Qi, Jie Song, Peng Liu, Yi Liu, Yun-Xiang Pan

《化学科学与工程前沿（英文）》 2020年 第14卷 第6期   页码 948-955 doi: 10.1007/s11705-020-1920-2

摘要： Cobalt hydroxide has been emerging as a promising catalyst for the electrocatalytic oxidation reactions, including the oxygen evolution reaction (OER) and glucose oxidation reaction (GOR). Herein, we prepared cobalt hydroxide nanoparticles (CoHP) and cobalt hydroxide nanosheets (CoHS) on nickel foam. In the electrocatalytic OER, CoHS shows an overpotential of 306 mV at a current density of 10 mA·cm . This is enhanced as compared with that of CoHP (367 mV at 10 mA·cm ). In addition, CoHS also exhibits an improved performance in the electrocatalytic GOR. The improved electrocatalytic performance of CoHS could be due to the higher ability of the two-dimensional nanosheets on CoHS in electron transfer. These results are useful for fabricating efficient catalysts for electrocatalytic oxidation reactions.

关键词： electrocatalytic oxidation     cobalt hydroxide     nanosheet     water     glucose    

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Synthesis and electrocatalytic property of cubic and spherical nanoparticles of cobalt platinum alloys

Xiaowei TENG, Hong YANG,

《化学科学与工程前沿（英文）》 2010年 第4卷 第1期   页码 45-51 doi: 10.1007/s11705-009-0308-0

摘要： This paper describes the morphological control and electrocatalytic property of CoPt nanoparticles. Both cubic and spherical CoPt nanoparticles were made using cobalt carbonyl and platinum 2,4-pentanedionate under different reaction temperatures in the presence of capping reagents, which included adamantanecarboxylic acid and hexadecylamine. Effects of heterogeneous species on shape of the CoPt nanoparticles were examined by replacing cobalt carbonyl with silver acetylacetonate. Our results suggest that the formation of different shapes of CoPt particles could be attributed to the affinity between cobalt and platinum, and the effects of capping agents. The size and shape dependent electrocatalytic properties of these nanoparticles were examined based on the direct methanol oxidation reaction.

关键词： spherical     2     4-pentanedionate     adamantanecarboxylic     acetylacetonate     electrocatalytic    

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A thermodynamic study of the removal of HCl and H

Joseph LEE, Bo FENG

《化学科学与工程前沿（英文）》 2012年 第6卷 第1期   页码 67-83 doi: 10.1007/s11705-011-1162-4

摘要： Advanced integrated-gasification combined-cycle (IGCC) and integrated-gasification fuel cell (IFGC) systems require high-temperature sorbents that are capable of removing hydrogen chloride and hydrogen sulfide from coal derived gases to very low levels. HCl and H S are highly reactive, corrosive, and toxic gases that must be removed to meet stringent environmental regulations, to protect power generation equipment and to control the emissions of contaminants. The thermodynamic behavior of 13 sorbents for the removal of HCl and H S under various conditions including: initial toxic gas concentration (1–10000 ppm), operating pressure (0.1–11 Mpa), temperature (300 K–1500 K), and the presence of H O were investigated. The correlation between HCl and H S was also examined. Thermodynamic calculations were carried out for the reactions of the 13 sorbents using a FactSage 5.2 software package based on free energy minimization. The sorbents, Na CO , NaHCO , K CO , and CaO are capable of completely removing chlorine at high temperatures (up to ~1240 K) and at high pressures. Water vapor did not have any significant effects on the dechlorination capability of the sorbents. Nine of the sorbents namely; Cu O, Na CO , NaHCO , K CO , CaO, ZnO, MnO, FeO, and PbO, were determined to have great potential as desulfurization sorbents. Cu O and ZnO had the best performance in terms of the optimum operating temperature. The addition of water vapor to the reactant gas produces a slightly detrimental effect on most of the sorbents, but FeO exhibited the worst performance with a reduction in the maximum operating temperature of about 428 K. The dechlorination performance of the alkali sorbents was not affected by the presence of H S in the reactions. However, the desulfurization capability of some sorbents was greatly affected by the presence of HCl. Particularly, the performance of Cu O was significantly reduced when HCl was present, but the performance of FeO improved remarkably. The thermodynamic results gathered are valuable for the developments of better sorbents.

关键词： syngas cleaning     sorbent     desulfurization     dechlorination    

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Overoxidized poly(3,4-ethylenedioxythiophene)-overoxidized polypyrrole composite films with enhanced electrocatalytic

《化学科学与工程前沿（英文）》 2023年 第17卷 第6期   页码 735-748 doi: 10.1007/s11705-022-2262-z

摘要： In this study, a simple and effective method was proposed to improve the electrocatalytic ability of overoxidized poly(3,4-ethylenedioxythiophene)-overoxidized polypyrrole composite films modified on glassy carbon electrode for rutin and luteolin determination. The composite electrode was prepared by cyclic voltammetry copolymerization with LiClO4-water as the supporting electrolyte. The peak current of rutin and luteolin on the composite electrode gradually decreased or even disappeared with the increase in the positive potential limit. After incubation in NaOH–ethanol solution with a volume ratio of 1:1, the composite electrodes prepared at positive potential limit greater than 1.5 V exhibited enhanced differential pulse voltammetry peak currents, reduced charge transfer resistance, larger effective specific surface area and higher electron transfer rate constant. The composite electrode prepared in the potential range of 0–1.7 V showed optimal electrocatalytic performance. The X-ray photoelectron spectroscopy results indicated that the content of –SO2/–SO and –C=N– groups in the composite film increased significantly after incubation. Further, the Raman spectra and Fourier transform infrared spectra revealed that the thiophene ring structure changed from benzene-type to quinone-type, and the quinone-type pyrrole ring was formed. The electrocatalytic mechanism of the composite film was proposed based on the experimental results and further verified by Density Functional Theory calculation.

关键词： overoxidized poly(3     4-ethylenedioxythiophene)-overoxidized polypyrrole     rutin     luteolin     incubation     electrocatalytic mechanism    

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Revisiting solar hydrogen production through photovoltaic-electrocatalytic and photoelectrochemical water

《能源前沿（英文）》 2021年 第15卷 第3期   页码 596-599 doi: 10.1007/s11708-021-0745-0

摘要： Photoelectrochemical (PEC) water splitting is regarded as a promising way for solar hydrogen production, while the fast development of photovoltaic-electrolysis (PV-EC) has pushed PEC research into an embarrassed situation. In this paper, a comparison of PEC and PV-EC in terms of efficiency, cost, and stability is conducted and briefly discussed. It is suggested that the PEC should target on high solar-to-hydrogen efficiency based on cheap semiconductors in order to maintain its role in the technological race of sustainable hydrogen production.

关键词： hydrogen production     photovoltaic     electrocatalysis     photoelectrocatalysis     water splitting    

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A 3D porous WP2 nanosheets@carbon cloth flexible electrode for efficient electrocatalytic hydrogen evolution

Mingyu Pi, Xiaodeng Wang, Dingke Zhang, Shuxia Wang, Shijian Chen

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 425-432 doi: 10.1007/s11705-018-1726-7

摘要：

Self-standing porous WP2 nanosheet arrays on carbon fiber cloth (WP2 NSs/CC) were synthesized and used as a 3D flexible hydrogen evolution electrode. Because of its 3D porous nanoarray structure, the WP2 NSs/CC exhibits a remarkable catalytic activity and a high stability. By using the experimental measurements and first-principle calculations, the underlying reasons for the excellent catalytic activity were further explored. Our work makes the present WP2 NSs as a promising electrocatalyst for hydrogen evolution and provides a way to design and fabricate efficient hydrogen evolution electrodes through 3D porous nano-arrays architecture.

关键词： WP2     nanosheet arrays     hydrogen evolution electrocatalyst     flexible electrode    

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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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Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reduction

Lin LI, Cehuang FU, Shuiyun SHEN, Fangling JIANG, Guanghua WEI, Junliang ZHANG

《能源前沿（英文）》 2022年 第16卷 第5期   页码 812-821 doi: 10.1007/s11708-020-0669-0

摘要： The development of highly active nitrogen-doped carbon-based transition metal (M-N-C) compounds for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs) greatly helps reduce fuel cell cost, thus rapidly promoting their commercial applications. Among different M-N-C electrocatalysts, the series of Fe-N-C materials are highly favored because of their high ORR activity. However, there remains a debate on the effect of Fe, and rare investigations focus on the influence of Fe addition in the second heat treatment usually performed after acid leaching in the catalyst synthesis. It is thus very critical to explore the influences of Fe on the ORR electrocatalytic activity, which will, in turn, guide the design of Fe-N-C materials with enhanced performance. Herein, a series of Fe-N-C electrocatalysts are synthesize and the influence of Fe on the ORR activity are speculated both experimentally and theoretically. It is deduced that the active site lies in the structure of Fe-N , accompanied with the addition of appropriate Fe, and the number of active sites increases without the occurrence of agglomeration particles. Moreover, it is speculated that Fe plays an important role in stabilizing N as well as constituting active sites in the second pyrolyzing process.

关键词： oxygen reduction reaction     Fe-N-C     active sites     Fe addition     second heat treatment    

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Dechlorination of 2,2′,4,4′,5,5′-hexachlorobiphenyl by thermal reaction with activated carbon-supported

Yifei SUN, Xin FU, Wei QIAO, Wei WANG, Tianle ZHU, Xinghua LI

《环境科学与工程前沿（英文）》 2013年 第7卷 第6期   页码 827-832 doi: 10.1007/s11783-013-0543-y

摘要： Activated carbon (AC)-supported copper or zinc made from ion exchange resin (IRCu-C and IRZn-C) have an increased metal load of 557.3 mg?g and 502.8 mg?g compared to those prepared by the traditional method involving impregnation with AC and copper (II) citrate or zinc citrate solution (LaCu-C and LaZn-C) of 12.9 mg?g and 46.0 mg?g respectively. When applied to decompose 2,2′,4,4′,5,5′-hexachlorobiphenyl at 250 °C, IRCu-C achieved higher activity of 99.0% decomposition efficiency than LaCu-C of 84.7%, IRZn-C of 90.5% and LaZn-C of 62.7%. When the reaction temperature rose to 350 °C, all the four kinds of reactants can decompose PCB-153 with efficiency above 90%. Further, X-ray photoelectron spectroscopy characterization of IRCu-C before and after the reaction indicated transformation of 19.1% of Cu atoms into Cu , illustrating that Cu is the active ingredient or electron donor promoting the decomposition of PCB-153. The mechanism underlying this process differs from a traditional H donor. However, there is no significant change on the surface of IRZn-C before and after the reaction, suggesting that Zn acts as catalyst during the process of PCB-153 decomposition.

关键词： polychlorinated biphenyls     activated carbon-supported copper or zinc     dechlorination     electron donor    

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标题 作者 时间 类型 操作

Efficient dechlorination of 2,4-dichlorophenol in an aqueous media with a mild pH using a Pd/TiO

Jiangkun DU,Jianguo BAO,Wei HU

期刊论文

Competition for electrons between reductive dechlorination and denitrification

Lifeng Cao, Weihua Sun, Yuting Zhang, Shimin Feng, Jinyun Dong, Yongming Zhang, Bruce E. Rittmann

期刊论文

Application of electrode materials and catalysts in electrocatalytic treatment of dye wastewater

期刊论文

Development and characterization of an anaerobic microcosm for reductive dechlorination of PCBs

Dawei Liang, Shanquan Wang

期刊论文

Multivalent manganese oxides with high electrocatalytic activity for oxygen reduction reaction

Xiangfeng Peng, Zhenhai Wang, Zhao Wang, Yunxiang Pan

期刊论文

Electrodeposited porous Pb electrode with improved electrocatalytic performance for the electroreduction

Jing WANG, Hua WANG, Zhenzhen HAN, Jinyu HAN

期刊论文

Noble-metal-free cobalt hydroxide nanosheets for efficient electrocatalytic oxidation

Jie Lan, Daizong Qi, Jie Song, Peng Liu, Yi Liu, Yun-Xiang Pan

期刊论文

Synthesis and electrocatalytic property of cubic and spherical nanoparticles of cobalt platinum alloys

Xiaowei TENG, Hong YANG,

期刊论文

A thermodynamic study of the removal of HCl and H

Joseph LEE, Bo FENG

期刊论文

Overoxidized poly(3,4-ethylenedioxythiophene)-overoxidized polypyrrole composite films with enhanced electrocatalytic

期刊论文

Revisiting solar hydrogen production through photovoltaic-electrocatalytic and photoelectrochemical water

期刊论文

A 3D porous WP2 nanosheets@carbon cloth flexible electrode for efficient electrocatalytic hydrogen evolution

Mingyu Pi, Xiaodeng Wang, Dingke Zhang, Shuxia Wang, Shijian Chen

期刊论文

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

期刊论文

Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reduction

Lin LI, Cehuang FU, Shuiyun SHEN, Fangling JIANG, Guanghua WEI, Junliang ZHANG

期刊论文

Dechlorination of 2,2′,4,4′,5,5′-hexachlorobiphenyl by thermal reaction with activated carbon-supported

Yifei SUN, Xin FU, Wei QIAO, Wei WANG, Tianle ZHU, Xinghua LI

期刊论文