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Adsorption performance and physicochemical mechanism of MnO

Xiaoyan Deng, Luxing Wang, Qihui Xiu, Ying Wang, Hong Han, Dongmei Dai, Yongji Xu, Hongtao Gao, Xien Liu

《化学科学与工程前沿（英文）》 2021年 第15卷 第3期   页码 538-551 doi: 10.1007/s11705-020-1958-1

摘要： In this work, an adsorbent, which we call MnPT, was prepared by combining MnO , polyethylenimine and tannic acid, and exhibited efficient performance for Cu(II) and Cr(VI) removal from aqueous solution. The oxygen/nitrogen-containing functional groups on the surface of MnPT might increase the enrichment of metal ions by complexation. The maximum adsorption capacities of MnPT for Cu(II) and Cr(VI) were 121.5 and 790.2 mg·g , respectively. The surface complexation formation model was used to elucidate the physicochemical interplay in the process of Cu(II) and Cr(VI) co-adsorption on MnPT. Electrostatic force, solvation action, adsorbate–adsorbate lateral interaction, and complexation were involved in the spontaneous adsorption process. Physical electrostatic action was dominant in the initial stage, whereas chemical action was the driving force leading to adsorption equilibrium. It should be noted that after adsorption on the surface of MnPT, Cr(VI) reacted with some reducing functional groups (hydroxylamine-NH ) and was converted into Cr(III). The adsorption capacity declined by 12% after recycling five times. Understanding the adsorption mechanism might provide a technical basis for the procedural design of heavy metal adsorbents. This MnPT nanocomposite has been proven to be a low-cost, efficient, and promising adsorbent for removing heavy metal ions from wastewater.

关键词： MnO2-polyethylenimine-tannic acid composite     surface complexation formation model     Cu(II)     Cr(VI)     physicochemical mechanism    

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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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All-inorganic TiO/CsAgBiBr composite as highly efficient photocatalyst under visible light irradiation

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 1925-1936 doi: 10.1007/s11705-023-2344-6

摘要： In recent years, limited photocatalysis efficiency and wide band gap have hindered the application of TiO2 in the field of photocatalysis. A leading star in photocatalysis has been revealed as lead-free Cs2AgBiBr6 double halide perovskite nanocrystals, owing to its strong visible light absorption and tunable band gap. In this work, this photocatalytic process was facilitated by a unique TiO2/Cs2AgBiBr6 composite, which was identified as an S-cheme heterojunction. TiO2/Cs2AgBiBr6 composite was investigated for its structure and photocatalytic behavior. The results showed that when the perovskite dosage is 40%, the photocatalytic rate of TiO2 could be boosted to 0.1369 min–1. This paper discusses and proposes the band gap matching, carrier separation, and photocatalytic mechanism of TiO2/Cs2AgBiBr6 composites, which will facilitate the generation of new ideas for improving TiO2’s photocatalytic performance.

关键词： Cs2AgBiBr6 nanocrystals     visible-light photocatalyst     Cs2AgBiBr6/TiO2 heterojunction    

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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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grown TiN/N-TiO composite for enhanced photocatalytic H evolution activity

《能源前沿（英文）》 2021年 第15卷 第3期   页码 721-731 doi: 10.1007/s11708-021-0766-8

摘要： Titanium nitride (TiN) decorated N-doped titania (N-TiO2) composite (TiN/N-TiO2) is fabricated via an in situ nitridation using a hydrothermally synthesized TiO2 and melamine (MA) as raw materials. After the optimization of the reaction condition, the resultant TiN/N-TiO2 composite delivers a hydrogen evolution activity of up to 703 μmol/h under the full spectrum irradiation of Xe-lamp, which is approximately 2.6 and 32.0 times more than that of TiO2 and TiN alone, respectively. To explore the underlying photocatalytic mechanism, the crystal phase, morphology, light absorption, energy band structure, element composition, and electrochemical behavior of the composite material are characterized and analyzed. The results indicate that the superior activity is mainly caused by the in situ formation of plasmonic TiN and N-TiO2 with intimate interface contact, which not only extends the spectral response range, but also accelerates the transfer and separation of the photoexcited hot charge carrier of TiN. The present study provides a fascinating approach to in situ forming nonmetallic plasmonic material/N-doped TiO2 composite photocatalysts for high-efficiency water splitting.

关键词： photocatalytic H2 evolution     TiN/N-TiO2 composite     plasmonic effect     in-situ nitridation    

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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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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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Ultrasound-assisted co-precipitation synthesis of mesoporous Co3O4–CeO2 composite oxides for highly selective

《化学科学与工程前沿（英文）》 2022年 第16卷 第8期   页码 1211-1223 doi: 10.1007/s11705-022-2145-3

摘要： The one-step highly selective oxidation of cyclohexane into cyclohexanone and cyclohexanol as the essential intermediates of nylon-6 and nylon-66 is considerably challenging. Therefore, an efficient and low-cost catalyst must be urgently developed to improve the efficiency of this process. In this study, a Co3O4–CeO2 composite oxide catalyst was successfully prepared through ultrasound-assisted co-precipitation. This catalyst exhibited a higher selectivity to KA-oil, which was benefited from the synergistic effects between Co3+/Co2+ and Ce4+/Ce3+ redox pairs, than bulk CeO2 and/or Co3O4. Under the optimum reaction conditions, 89.6% selectivity to KA-oil with a cyclohexane conversion of 5.8% was achieved over Co3O4–CeO2. Its catalytic performance remained unchanged after five runs. Using the synergistic effects between the redox pairs of different transition metals, this study provides a feasible strategy to design high-performance catalysts for the selective oxidation of alkanes.

关键词： Co3O4–CeO2 composite oxides     cyclohexanone     cyclohexanol     ultrasonic-assisted co-precipitation     selective oxidation     solvent-free    

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Effect of different acid anions on highly efficient Ce-based catalysts for selective catalytic reductionof NO with NH<sub>3sub>

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1399-1411 doi: 10.1007/s11705-023-2345-5

摘要： Three kinds of Ce-based catalysts (CePO4, CeVO4, Ce2(SO4)3) were synthesized and used for the selective catalytic reduction (SCR) of NO by NH3. NH3-SCR performances were conducted in the temperature range of 80 to 400 °C. The catalytic efficiencies of the three catalysts are as follow: CePO4 > CeVO4 > Ce2(SO4)3, which is in agreement with their abilities of NH3 adsorption capacities. The highest NO conversion rate of CePO4 could reach about 95%, and the catalyst had more than 90% NO conversion rate between 260 and 320 °C. The effect of PO43–, VO43– and SO42– on NH3-SCR performances of Ce-based catalysts was systematically investigated by the X-ray photoelectron spectroscopy analysis, NH3 temperature programmed desorption, H2 temperature programmed reduction and field emission scanning electron microscopy tests. The key factors that can enhance the SCR are the existence of Ce4+, large NH3 adsorption capacity, high and early H2 consumptions, and suitable microstructures for gas adsorption. Finally, CePO4 and CeVO4 catalysts also exhibited relatively strong tolerance of SO2, and the upward trend about 8% was detected due to the sulfation enhancement by SO2 for Ce2(SO4)3.

关键词： CePO4     CeVO4     Ce2(SO4)3     selective catalytic reduction     NO removal    

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Chemical deactivation of V

Xiaodong WU, Wenchao YU, Zhichun SI, Duan WENG

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 420-427 doi: 10.1007/s11783-013-0489-0

摘要： V O -WO /TiO catalyst was poisoned by impregnation with NH Cl, KOH and KCl solution, respectively. The catalysts were characterized by X-ray diffraction (XRD), inductively coupled plasma (ICP), N physisorption, Raman, UV-vis, NH adsorption, temperature-programmed reduction of hydrogen (H -TPR), temperature-programmed oxidation of ammonia (NH -TPO) and selective catalytic reduction of NO with ammonia (NH -SCR). The deactivation effects of poisoning agents follow the sequence of KCl>KOH>>NH Cl. The addition of ammonia chloride enlarges the pore size of the titania support, and promotes the formation of highly dispersed V=O vanadyl which improves the oxidation of ammonia and the high-temperature SCR activity. K ions are suggested to interact with vanadium and tungsten species chemically, resulting in a poor redox property of catalyst. More importantly, potassium can reduce the Br?nsted acidity of catalysts and decrease the stability of Br?nsted acid sites significantly. The more severe deactivation of the KCl-treated catalyst can be mainly ascribed to the higher amount of potassium resided on catalyst.

关键词： V2O5-WO3/TiO2     potassium chloride     poisoning     reducibility     acid sites    

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NiCo2O4@quinone-rich N–C core–shell nanowires as composite electrode for electric double layer capacitor

《化学科学与工程前沿（英文）》 2023年 第17卷 第4期   页码 373-386 doi: 10.1007/s11705-022-2223-6

摘要： The bind-free carbon cloth-supported electrodes hold the promises for high-performance electrochemical capacitors with high specific capacitance and good cyclic stability. Considering the close connection between their performance and the amount of carbon material loaded on the electrodes, in this work, NiCo2O4 nanowires were firstly grown on the substrate of active carbon cloth to provide the necessary surface area in the longitudinal direction. Then, the quinone-rich nitrogen-doped carbon shell structure was formed around NiCo2O4 nanowires, and the obtained composite was used as electrode for electric double layer capacitor. The results showed that the composite electrode displayed an area-specific capacitance of 1794 mF∙cm–2 at the current density of 1 mA∙cm–2. The assembled symmetric electric double layer capacitor achieved a high energy density of 6.55 mW∙h∙cm–3 at a power density of 180 mW∙cm–3. The assembled symmetric capacitor exhibited a capacitance retention of 88.96% after 10000 charge/discharge cycles at the current density of 20 mA∙cm–2. These results indicated the potentials in the preparation of the carbon electrode materials with high energy density and good cycling stability.

关键词： carbon cloth     NiCo2O4 nanowires     core−shell structure     quinone-rich     electric double layer capacitor    

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Molecular level understanding of CO<sub>2sub> capture in ionic liquid/polyimide composite membrane

Linlin You, Yandong Guo, Yanjing He, Feng Huo, Shaojuan Zeng, Chunshan Li, Xiangping Zhang, Xiaochun Zhang

《化学科学与工程前沿（英文）》 2022年 第16卷 第2期   页码 141-151 doi: 10.1007/s11705-020-2009-7

摘要： Ionic liquid (IL)/polyimide (PI) composite membranes demonstrate promise for use in CO separation applications. However, few studies have focused on the microscopic mechanism of CO in these composite systems, which is important information for designing new membranes. In this work, a series of systems of CO in 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide composited with 4,4-(hexafluoroisopropylidene) diphthalic anhydride (6FDA)-based PI, 6FDA-2,3,5,6-tetramethyl-1,4-phenylene-diamine, at different IL concentrations were investigated by all-atom molecular dynamics simulation. The formation of IL regions in PI was found, and the IL regions gradually became continuous channels with increasing IL concentrations. The analysis of the radial distribution functions and hydrogen bond numbers demonstrated that PI had a stronger interaction with cations than anions. However, the hydrogen bonds among PI chains were destroyed by the addition of IL, which was favorable for transporting CO . Furthermore, the self-diffusion coefficient and free energy barrier suggested that the diffusion coefficient of CO decreased with increasing IL concentrations up to 35 wt-% due to the decrease of the fractional free volume of the composite membrane. However, the CO self-diffusion coefficients increased when the IL contents were higher than 35 wt-%, which was attributed to the formation of continuous IL domain that benefitted the transportation of CO .

关键词： carbon dioxide     ionic liquid     6FDA-TeMPD     composite membrane     molecular dynamics simulation    

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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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标题 作者 时间 类型 操作

Adsorption performance and physicochemical mechanism of MnO

Xiaoyan Deng, Luxing Wang, Qihui Xiu, Ying Wang, Hong Han, Dongmei Dai, Yongji Xu, Hongtao Gao, Xien Liu

期刊论文

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

All-inorganic TiO/CsAgBiBr composite as highly efficient photocatalyst under visible light irradiation

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

grown TiN/N-TiO composite for enhanced photocatalytic H evolution activity

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

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

Ultrasound-assisted co-precipitation synthesis of mesoporous Co3O4–CeO2 composite oxides for highly selective

期刊论文

Effect of different acid anions on highly efficient Ce-based catalysts for selective catalytic reductionof NO with NH<sub>3sub>

期刊论文

Chemical deactivation of V

Xiaodong WU, Wenchao YU, Zhichun SI, Duan WENG

期刊论文

NiCo2O4@quinone-rich N–C core–shell nanowires as composite electrode for electric double layer capacitor

期刊论文

Molecular level understanding of CO<sub>2sub> capture in ionic liquid/polyimide composite membrane

Linlin You, Yandong Guo, Yanjing He, Feng Huo, Shaojuan Zeng, Chunshan Li, Xiangping Zhang, Xiaochun Zhang

期刊论文

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

期刊论文