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Catalytic activities and mechanism of formaldehyde oxidation over gold supported on MnO

Guanglong PANG,Donghui WANG,Yunhong ZHANG,Chunyan MA,Zhengping HAO

《环境科学与工程前沿（英文）》 2016年 第10卷 第3期   页码 447-457 doi: 10.1007/s11783-015-0808-8

摘要： MnO microspheres with various surface structures were prepared using the hydrothermal method, and Au/MnO catalysts were synthesized using the sol-gel method. We obtained three MnO microspheres and Au/MnO samples: coherent solid spheres covered with wire-like nanostructures, solid spheres with nanosheets, and hierarchical hollow microspheres with nanoplatelets and nanorods. We investigated the properties and catalytic activities of formaldehyde oxidation at room temperature. Crystalline structures of MnO are the main factor affecting the catalytic activities of these samples, and γ-MnO shows high catalytic performance. The excellent redox properties are responsible for the catalytic ability of γ-MnO . The gold-supported interaction can change the redox properties of catalysts and accelerate surface oxygen species transition, which can account for the catalytic activity enhancement of Au/MnO . We also studied intermediate species. The dioxymethylene (DOM) and formate species formed on the catalyst surface were considered intermediates, and were ultimately transformed into hydrocarbonate and carbonate and then decomposed into CO . A proposed mechanism of formaldehyde oxidation over Au/MnO catalysts was also obtained.

关键词： MnO2 microspheres     Au/MnO2     formaldehyde oxidation     γ-MnO2    

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g-CN-coated MnO hollow nanorod cathode for stable aqueous Zn-ion batteries

《化学科学与工程前沿（英文）》 2023年 第17卷 第2期   页码 217-225 doi: 10.1007/s11705-022-2214-7

摘要： Aqueous zinc-ion batteries are attracting considerable attention because of their high safety compared with conventional lithium-ion batteries. Manganese-based materials have been widely developed for zinc-ion batteries cathode owning to their low cost, high security and simple preparation. However, the severe volume expansion and poor stability during charging and discharging limit the further development of manganese-based cathodes. Herein, superior α-MnO2@g-C3N4 was successfully prepared for stable zinc-ion batteries (ZIBs) cathode by introducing g-C3N4 nanosheets. Compared with pure α-MnO2, α-MnO2@g-C3N4 has a specific capacity of 298 mAh·g–1 at 0.1 A·g–1. Even at 1 A·g–1, the α-MnO2@g-C3N4 still retains 100 mAh·g–1 (83.4% retention after 5000 cycles), implying its excellent cycling stability. The α-MnO2@g-C3N4-based cathode has the highest energy density (563 Wh·kg–1) and power energy density (2170 W·kg–1). This work provides new avenues for the development of a wider range of cathode materials for ZIBs.

关键词： α-MnO2 hollow nanorods     g-C3N4     heterojunction     aqueous Zn-ion batteries    

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Preparation of biomass-derived carbon loaded with MnO as lithium-ion battery anode for improving its

《化学科学与工程前沿（英文）》 2023年 第18卷 第1期 doi: 10.1007/s11705-023-2376-y

摘要： Biomass-derived carbon materials for lithium-ion batteries emerge as one of the most promising anodes from sustainable perspective. However, improving the reversible capacity and cycling performance remains a long-standing challenge. By combining the benefits of K2CO3 activation and KMnO4 hydrothermal treatment, this work proposes a two-step activation method to load MnO2 charge transfer onto biomass-derived carbon (KAC@MnO2). Comprehensive analysis reveals that KAC@MnO2 has a micro-mesoporous coexistence structure and uniform surface distribution of MnO2, thus providing an improved electrochemical performance. Specifically, KAC@MnO2 exhibits an initial charge-discharge capacity of 847.3/1813.2 mAh·g–1 at 0.2 A·g–1, which is significantly higher than that of direct pyrolysis carbon and K2CO3 activated carbon, respectively. Furthermore, the KAC@MnO2 maintains a reversible capacity of 652.6 mAh·g–1 after 100 cycles. Even at a high current density of 1.0 A·g–1, KAC@MnO2 still exhibits excellent long-term cycling stability and maintains a stable reversible capacity of 306.7 mAh·g–1 after 500 cycles. Compared with reported biochar anode materials, the KAC@MnO2 prepared in this work shows superior reversible capacity and cycling performance. Additionally, the Li+ insertion and de-insertion mechanisms are verified by ex situ X-ray diffraction analysis during the charge-discharge process, helping us better understand the energy storage mechanism of KAC@MnO2.

关键词： biomass-derived carbon     MnO2     lithium-ion batteries     anode material     high reversible capacity    

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Facile synthesis of α-MnO

Weixin ZHANG, Wenran ZHAO, Zaoyuan ZHOU, Zeheng YANG

《化学科学与工程前沿（英文）》 2014年 第8卷 第1期   页码 64-72 doi: 10.1007/s11705-014-1402-5

摘要： In this paper, α-MnO micronests composed of nanowires were fabricated via a hydrothermal reaction of MnSO ·H O and K S O solutions. The α-MnO micronests were demonstrated to have a higher adsorption capacity than γ-MnO microspheres due to their large specific surface area. The amount of Congo red adsorbed per unit weight of α-MnO micronests increased significantly from 114 to 282 mg·g with concentration of Congo red solution increasing from 50 to 200 mg·L , but it had a little change with temperature. Kinetics, isotherms and thermodynamics for the adsorption of Congo red on α-MnO micronests were examined. The adsorption process followed the pseudo-second-order kinetics with good correlation. The experimental data were analyzed by Langmuir and Freundlich models, and equilibrium data fitted the Langmuir isotherm very well with maximum monolayer adsorption capacity of 625 mg·g at 22 °C. The adsorption was spontaneous and endothermic according to thermodynamic studies. The experimental results indicate that α-MnO micronests possess a high adsorption capacity and could be employed as a replacement of traditional sorbents.

关键词： MnO2     Congo red     adsorption     kinetics     isotherm     thermodynamics    

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Co-present Pb(II) accelerates the oxidation of organic contaminants by permanganate: Role of Pb(III)

《环境科学与工程前沿（英文）》 2022年 第16卷 第8期 doi: 10.1007/s11783-022-1530-y

摘要：

• Simultaneous removal of organic contaminants and Pb(II) was achieved by Mn(VII).

关键词： Permanganate     Pb(II) oxidation     MnO2     pH effect    

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Effects of oxidizing environment on digestate humification and identification of substances governing the dissolved organic matter (DOM) transformation process

《环境科学与工程前沿（英文）》 2022年 第16卷 第8期 doi: 10.1007/s11783-022-1520-0

摘要：

• Liquid digestate humification was investigated under different oxidizing environment.

关键词： Liquid digestate     MnO2     Oxygen     DOM transformation     Humic-like acids    

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Reduction kinetics of SrFeO/CaO∙MnO nanocomposite as effective oxygen carrier for chemical looping partial

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1726-1734 doi: 10.1007/s11705-022-2188-5

摘要： Chemical looping reforming of methane is a novel and effective approach to convert methane to syngas, in which oxygen transfer is achieved by a redox material. Although lots of efforts have been made to develop high-performance redox materials, a few studies have focused on the redox kinetics. In this work, the kinetics of SrFeO3−δ–CaO∙MnO nanocomposite reduction by methane was investigated both on a thermo-gravimetric analyzer and in a packed-bed microreactor. During the methane reduction, combustion occurs before the partial oxidation and there exists a transition between them. The weight loss due to combustion increases, but the transition region becomes less inconspicuous as the reduction temperature increased. The weight loss associated with the partial oxidation is much larger than that with combustion. The rate of weight loss related to the partial oxidation is well fitted by the Avrami–Erofeyev equation with n = 3 (A3 model) with an activation energy of 59.8 kJ∙mol‒1. The rate law for the partial oxidation includes a solid conversion term whose expression is given by the A3 model and a methane pressure-dependent term represented by a power law. The partial oxidation is half order with respect to methane pressure. The proposed rate law could well predict the reduction kinetics; thus, it may be used to design and/or analyze a chemical looping reforming reactor.

关键词： chemical looping reforming     SrFeO3−δ/CaO·MnO nanocomposite     reduction kinetics     Avrami–Erofeyev model     pressure-dependent term    

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Denitrification performance and sulfur resistance mechanism of Sm–Mn catalyst for low temperature NH-SCR

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 617-633 doi: 10.1007/s11705-022-2258-8

摘要： MnOx and Sm–Mn catalysts were prepared with the coprecipitation method, and they showed excellent activities and sulfur resistances for the selective catalytic reduction of NOx by NH3 between 50 and 300 °C in the presence of excess oxygen. 0.10Sm–Mn catalyst indicated better catalytic activity and sulfur resistance. Additionally, the Sm doping led to multi-aspect impacts on the phases, morphology structures, gas adsorption, reactions process, and specific surface areas. Therefore, it significantly enhances the NO conversion, N2 selectivity, and sulfur resistance. Based on various experimental characterization results, the reaction mechanism of catalysts and the effect of SO2 on the reaction process about the catalysts were extensively explored. For 0.10Sm–Mn catalyst, manganese sulfate and sulfur ammonium cannot be generated broadly under the influence of SO2 and the amount of surface adsorbed oxygen. The Bronsted acid sites strengthen significantly due to the addition of SO2, enhancing the sulfur resistance of the 0.10Sm–Mn catalyst.

关键词： MnOx     Sm–Mn     catalyst     NH3-SCR     sulfur resistance    

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Rh<sub>2sub>O<sub>3sub>/hexagonal CePO<sub>4sub> nanocatalysts for N<sub>2sub>O decomposition

Huan Liu, Zhen Ma

《化学科学与工程前沿（英文）》 2017年 第11卷 第4期   页码 586-593 doi: 10.1007/s11705-017-1659-6

摘要： Hexagonal CePO nanorods were prepared by a precipitation method and hexagonal CePO nanowires were prepared by hydrothermal synthesis at 150 °C. Rh(NO ) was then used as a precursor for the impregnation of Rh O onto these CePO materials. The Rh O supported on the CePO nanowires was much more active for the catalytic decomposition of N O than the Rh O supported on CePO nanorods. The stability of both catalysts as a function of time on stream was studied and the influence of the co-feed (CO , O , H O or O /H O) on the N O decomposition was also investigated. The samples were characterized by N adsorption-desorption, inductively coupled plasma optical emission spectroscopy, X-ray diffraction, transmission electron microscopy, X-ray photoelectron microscopy, hydrogen temperature-programmed reduction, oxygen temperature-programmed desorption, and CO temperature-programmed desorption in order to correlate the physicochemical and catalytic properties.

关键词： Rh2O3     CePO4     N2O decomposition    

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CO<sub>2sub> methanation and co-methanation of CO and CO<sub>2sub> over Mn-promoted Ni/Al<sub>2sub>O<sub>3sub> catalysts

Kechao Zhao,Zhenhua Li,Li Bian

《化学科学与工程前沿（英文）》 2016年 第10卷 第2期   页码 273-280 doi: 10.1007/s11705-016-1563-5

摘要： A series of Mn-promoted 15 wt-% Ni/Al O catalysts were prepared by an incipient wetness impregnation method. The effect of the Mn content on the activity of the Ni/Al O catalysts for CO methanation and the co-methanation of CO and CO in a fixed-bed reactor was investigated. The catalysts were characterized by N physisorption, hydrogen temperature-programmed reduction and desorption, carbon dioxide temperature-programmed desorption, X-ray diffraction and high-resolution transmission electron microscopy. The presence of Mn increased the number of CO adsorption sites and inhibited Ni particle agglomeration due to improved Ni dispersion and weakened interactions between the nickel species and the support. The Mn-promoted 15 wt-% Ni/Al O catalysts had improved CO methanation activity especially at low temperatures (250 to 400 °C). The Mn content was varied from 0.86% to 2.54% and the best CO conversion was achieved with the 1.71Mn-Ni/Al O catalyst. The co-methanation tests on the 1.71Mn-Ni/Al O catalyst indicated that adding Mn markedly enhanced the CO methanation activity especially at low temperatures but it had little influence on the CO methanation performance. CO methanation was more sensitive to the reaction temperature and the space velocity than the CO methanation in the co-methanation process.

关键词： Mn promotion     nickel catalysts     CO2 methanation     co-methanation of CO and CO2    

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以净零排放为目标的封存驱动型CO<sub>2sub>提高采收率方法 Article

刘月亮, 芮振华

《工程（英文）》 2022年 第18卷 第11期   页码 79-87 doi: 10.1016/j.eng.2022.02.010

摘要： 可通过驱油过程将CO<sub>2sub>封存在油藏地质体中，因此，CO<sub>2sub>驱油与封存被视为降低CO<sub>2sub>排放的重要手段之一。本研究提出了一种新型的CO<sub>2sub>提高采收率（EOR）方法，即封存驱动型CO<sub>2sub>提高采收率，其主要目标是通过在油藏中封存尽可能多的CO<sub>2sub>来实现CO结果表明，DME可提高CO<sub>2sub>在原油中的溶解度，有利于CO<sub>2sub>的溶解封存；可抑制因CO<sub>2sub>的抽提作用造成的原油轻质组分“逃逸&rdquo封存驱动型CO<sub>2sub> EOR方法在提高波及效率方面优于传统的CO<sub>2sub> EOR，尤其是在采油后期更为明显；同时，封存驱动型CO<sub>2sub> EOR比传统的此外，通过封存驱动型CO<sub>2sub> EOR封存的CO<sub>2sub>量远超采出原油燃烧产生的碳排放总量。

关键词： CO<sub>2sub> EOR     CO<sub>2sub>净排放量     二甲醚     封存驱动型CO<sub>2sub> EOR     CO<sub>2sub>封存    

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Al<sub>2sub>O<sub>3sub> and CeO<sub>2sub>-promoted MgO sorbents for CO<sub>2sub> capture at moderate

Huimei Yu, Xiaoxing Wang, Zhu Shu, Mamoru Fujii, Chunshan Song

《化学科学与工程前沿（英文）》 2018年 第12卷 第1期   页码 83-93 doi: 10.1007/s11705-017-1691-6

摘要： A series of Al O and CeO modified MgO sorbents was prepared and studied for CO sorption at moderate temperatures. The CO sorption capacity of MgO was enhanced with the addition of either Al O or CeO . Over Al O -MgO sorbents, the best capacity of 24.6 mg-CO /g-sorbent was attained at 100 °C, which was 61% higher than that of MgO (15.3 mg-CO /g-sorbent). The highest capacity of 35.3 mg-CO /g-sorbent was obtained over the CeO -MgO sorbents at the optimal temperature of 200 °C. Combining with the characterization results, we conclude that the promotion effect on CO sorption with the addition of Al O and CeO can be attributed to the increased surface area with reduced MgO crystallite size. Moreover, the addition of CeO increased the basicity of MgO phase, resulting in more increase in the CO capacity than Al O promoter. Both the Al O -MgO and CeO -MgO sorbents exhibited better cyclic stability than MgO over the course of fifteen CO sorption-desorption cycles. Compared to Al O , CeO is more effective for promoting the CO capacity of MgO. To enhance the CO capacity of MgO sorbent, increasing the basicity is more effective than the increase in the surface area.

关键词： CO2 capture     MgO sorbents     Al2O3     CeO2     flue gas    

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ZnFe<sub>2sub>O<sub>4sub> deposited on BiOCl with exposed (001) and (010) facets for photocatalyticreduction of CO<sub>2sub> in cyclohexanol

Guixian Song, Xionggang Wu, Feng Xin, Xiaohong Yin

《化学科学与工程前沿（英文）》 2017年 第11卷 第2期   页码 197-204 doi: 10.1007/s11705-016-1606-y

摘要： ZnFe O -BiOCl composites were prepared by both hydrothermal and direct precipitation processes and the structures and properties of the samples were characterized by various instrumental techniques. The samples were then used as catalysts for the photocatalytic reduction of CO in cyclohexanol under ultraviolet irradiation to give cyclohexanone (CH) and cyclohexyl formate (CF). The photocatalytic CO reduction activities over the hydrothermally prepared ZnFe O -BiOCl composites were higher than those over the directly-precipitated composites. This is because compared to the direct-precipitation sample, the ZnFe O nanoparticles in the hydrothermal sample were smaller and more uniformly distributed on the surface of BiOCl and so more heterojunctions were formed. Higher CF and CH yields were obtained for the pure BiOCl and BiOCl composite samples with more exposed (001) facets than for the samples with more exposed (010) facets. This is due to the higher density of oxygen atoms in the exposed (001) facets, which creates more oxygen vacancies, and thereby improves the separation efficiency of the electron-hole pairs. More importantly, irradiation of the (001) facets with ultraviolet light produces photo-generated electrons which is helpful for the reduction of CO to ·CO . The mechanism for the photocatalytic reduction of CO in cyclohexanol over ZnFe O -BiOCl composites with exposed (001) facets involves electron transfer and carbon radical formation.

关键词： reduction of CO2     cyclohexanol     ZnFe2O4 deposited BiOCl     facet     composite photocatalyst    

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The stabilization effect of Al<sub>2sub>O<sub>3sub> on unconventional Pb/SiO<sub>2sub> catalyst

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1423-1429 doi: 10.1007/s11705-023-2315-y

摘要： Similar to Sn, Pb located at the same group (IVA) in the periodic table of elements, can also catalyze propane dehydrogenation to propene, while a fast deactivation can be observed. To enhance the stability, the traditional carrier Al2O3 with a small amount, was introduced into Pb/SiO2 catalyst in this study. It has been proved that Al2O3 can inhibit the reduction of PbO, and weaken the agglomeration and loss of Pb species due to its enhanced interaction with Pb species. As a result, 3Al15Pb/SiO2 catalyst exhibits a much higher stability up to more than 150 h. In addition, a simple schematic diagram of the change of surface species on the catalyst surface after Al2O3 addition was also proposed.

关键词： Pb/SiO2     Al2O3     propane dehydrogenation     propene     stability    

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Cu-doped Bi/Bi<sub>2sub>WO<sub>6sub> catalysts for efficient N<sub>2sub> fixation by photocatalysis

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1412-1422 doi: 10.1007/s11705-023-2312-1

摘要： In this paper, Cu-doped Bi2WO6 was synthesized via a solvothermal method and applied it in photocatalytic N2 immobilization. Characterization results showed the presence of a small amount of metallic Bi in the photocatalyst, indicating that the synthesized photocatalyst is actually Bi/Cu-Bi2WO6 composite. The doped Cu had a valence state of +2 and most likely substituted the position of Bi3+. The introduced Cu did not affect the metallic Bi content, but mainly influenced the energy band structure of Bi2WO6. The band gap was slightly narrowed, the conduction band was elevated, and the work function was reduced. The reduced work function improved the transfer and separation of charge carriers, which mainly caused the increased photoactivity. The optimized NH3 generation rates of Bi/Cu-Bi2WO6 reached 624 and 243 μmol·L–1·g–1·h–1 under simulated solar and visible light, and these values were approximately 2.8 and 5.9 times higher those of Bi/Bi2WO6, respectively. This research provides a method for improving the photocatalytic N2 fixation and may provide more information on the design and preparation of heteroatom-doped semiconductor photocatalysts for N2-to-NH3 conversion.

关键词： Bi2WO6     Cu doping     work function     photocatalytic N2 fixation     charge separation    

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标题 作者 时间 类型 操作

Catalytic activities and mechanism of formaldehyde oxidation over gold supported on MnO

Guanglong PANG,Donghui WANG,Yunhong ZHANG,Chunyan MA,Zhengping HAO

期刊论文

g-CN-coated MnO hollow nanorod cathode for stable aqueous Zn-ion batteries

期刊论文

Preparation of biomass-derived carbon loaded with MnO as lithium-ion battery anode for improving its

期刊论文

Facile synthesis of α-MnO

Weixin ZHANG, Wenran ZHAO, Zaoyuan ZHOU, Zeheng YANG

期刊论文

Co-present Pb(II) accelerates the oxidation of organic contaminants by permanganate: Role of Pb(III)

期刊论文

Effects of oxidizing environment on digestate humification and identification of substances governing the dissolved organic matter (DOM) transformation process

期刊论文

Reduction kinetics of SrFeO/CaO∙MnO nanocomposite as effective oxygen carrier for chemical looping partial

期刊论文

Denitrification performance and sulfur resistance mechanism of Sm–Mn catalyst for low temperature NH-SCR

期刊论文

Rh<sub>2sub>O<sub>3sub>/hexagonal CePO<sub>4sub> nanocatalysts for N<sub>2sub>O decomposition

Huan Liu, Zhen Ma

期刊论文

CO<sub>2sub> methanation and co-methanation of CO and CO<sub>2sub> over Mn-promoted Ni/Al<sub>2sub>O<sub>3sub> catalysts

Kechao Zhao,Zhenhua Li,Li Bian

期刊论文

以净零排放为目标的封存驱动型CO<sub>2sub>提高采收率方法

刘月亮, 芮振华

期刊论文

Al<sub>2sub>O<sub>3sub> and CeO<sub>2sub>-promoted MgO sorbents for CO<sub>2sub> capture at moderate

Huimei Yu, Xiaoxing Wang, Zhu Shu, Mamoru Fujii, Chunshan Song

期刊论文

ZnFe<sub>2sub>O<sub>4sub> deposited on BiOCl with exposed (001) and (010) facets for photocatalyticreduction of CO<sub>2sub> in cyclohexanol

Guixian Song, Xionggang Wu, Feng Xin, Xiaohong Yin

期刊论文

The stabilization effect of Al<sub>2sub>O<sub>3sub> on unconventional Pb/SiO<sub>2sub> catalyst

期刊论文

Cu-doped Bi/Bi<sub>2sub>WO<sub>6sub> catalysts for efficient N<sub>2sub> fixation by photocatalysis

期刊论文