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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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Enhanced heterogeneous Fenton-like activity by Cu-doped BiFeO

Jie Mao, Xie Quan, Jing Wang, Cong Gao, Shuo Chen, Hongtao Yu, Yaobin Zhang

《环境科学与工程前沿（英文）》 2018年 第12卷 第6期 doi: 10.1007/s11783-018-1060-9

摘要：

OH played a key role in heterogeneous Fenton-like catalytic oxidation of organic pollutants.

Doping Cu into BiFeO3 promoted the generation of Fe2+ and then facilitated the effective formation of •OH.

Cu-doped BiFeO3 exhibited higher catalytic performance for phenol degradation than non-doped BiFeO3.

关键词： Cu doped BiFeO3     Heterogeneous Fenton-like catalysts     Oxidative degradation    

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Cu-doped Bi/Bi2WO6 catalysts for efficient N2 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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Hydrothermal synthesis of crystalline α-/β-MnO2 nanorods via γ-MnOOH nanorod precursors

ZHANG Weixin, REN Xiangbin, YANG Zeheng, WANG Hua, WANG Qiang, HUANG Fei

《化学科学与工程前沿（英文）》 2007年 第1卷 第4期   页码 365-371 doi: 10.1007/s11705-007-0066-9

摘要： The crystalline -MnO and -MnO nanorods have been successfully prepared via a facile hydrothermal method from -MnOOH nanorods precursor, respectively. The samples were characterized by means of X-ray diff raction (XRD), transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), field emission scanning electron microscope (FESEM) and Fourier transformed infrared spectra (FTIR). The morphology and structure of -MnOOH nanorods precursors have a great influence on the crystal structure of the obtained products. The -MnO nanorods are prepared from the 100°C -MnOOH precursor, while the -MnO nanorods are obtained from the 150°C -MnOOH precursor, respectively. Besides, the catalytic activity of the prepared -MnO and -MnO nanorods for the HO decomposition has been investigated comparatively, and the latter shows better catalytic activity.

关键词： obtained     -MnOOH precursor     Besides     high-resolution transmission     precursor    

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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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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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Atomic force microscopy study on the microtopography of natural organic matter and newly formed hydrous MnO2

GUO Jin, MA Jun, SHI Xuehua

《环境科学与工程前沿（英文）》 2007年 第1卷 第2期   页码 251-256 doi: 10.1007/s11783-007-0043-z

摘要： To understand the water purification mechanism of potassium permanganate as a coagulation-aid during the preoxidation process, the microtopography of its reductive products, the newly formed hydrous manganese dioxide and the aged hydrous manganese dioxide, was investigated. The morphology of natural organic matter (NOM) adsorbed by the newly formed hydrous manganese dioxide was also compared with that of NOM alone. By using the tapping mode atomic force microscopy (AFM), the observation results show that the newly formed hydrous manganese dioxide possess a perforated sheet (with a thickness of 0 1.75 nm) as well as some spherical particle structures compared with the hydrous manganese dioxide with 2 h aging time, which demonstrated that the newly formed hydrous manganese dioxide had a large surface area and adsorption capacity. When 1 mmol/L newly formed hydrous manganese dioxide was added, the microtopography of NOM molecules shifted from a loosely dispersed pancake shape (with adsorption height of 5 8.5 nm) to a densely dispersed and uniform spherical structure. These results provide a valid proof that it is the perfect adsorption capability of the newly formed hydrous manganese dioxide that might result in the coagulation aid effect of potassium permanganate preoxidation.

关键词： spherical     microtopography     potassium permanganate     uniform spherical     morphology    

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Preparation and investigation of Pd doped Cu catalysts for selective hydrogenation of acetylene

Xinxiang Cao, Tengteng Lyu, Wentao Xie, Arash Mirjalili, Adelaide Bradicich, Ricky Huitema, Ben W.-L. Jang, Jong K. Keum, Karren More, Changjun Liu, Xiaoliang Yan

《化学科学与工程前沿（英文）》 2020年 第14卷 第4期   页码 522-533 doi: 10.1007/s11705-019-1822-3

摘要： A series of PdCu bimetallic catalysts with low Cu and Pd loadings and different Cu: Pd atomic ratios were prepared by conventionally sequential impregnation (CSI) and modified sequential impregnation (MSI) of Cu and Pd for selective hydrogenation of acetylene. Characterization indicates that the supported copper (II) nitrate in the PdCu bimetallic catalysts prepared by MSI can be directly reduced to Cu metal particles due to the hydrogen spillover from Pd to Cu(NO ) crystals. In addition, for the catalysts prepared by MSI, Pd atoms can form PdCu alloy on the surface of metal particles, however, for the catalysts prepared by CSI, Pd tends to migrate and exist below the surface layer of Cu. Reaction results indicate that compared with CSI, the MSI method enables samples to possess preferable stability as well as comparable reaction activity. This should be due to the MSI method in favor of the formation of PdCu alloy on the surface of metal particles. Moreover, even Pd loading is super low,<0.045 wt-% in this study, by through adjusting Cu loading to an appropriate value, attractive reactivity and selectivity still can be achieved.

关键词： copper     palladium     catalysts     acetylene     selective hydrogenation    

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Preparation of Cu/ZrO

Xinmei LIU, Shaofen BAI, Huidong ZHUANG, Zifeng YAN

《化学科学与工程前沿（英文）》 2012年 第6卷 第1期   页码 47-52 doi: 10.1007/s11705-011-1170-4

摘要： Cu/ZrO catalysts for methanol synthesis from CO /H were respectively prepared by deposition coprecipitation (DP) and solid state reaction (SR) methods. There is an intimate interaction between copper and zirconia, which strongly affects the reduction property and catalytic performance of the catalysts. The stronger the interaction, the lower the reduction temperature and the better the performance of the catalysts. Surface area, pore structure and crystal structure of the catalysts are mainly controlled by preparation methods and alkalinity of synthesis system. The conversion of CO and selectivity of methanol are higher for DP catalysts than for SP catalysts.

关键词： Cu/ZrO2     methanol synthesis     deposition coprecipitation     solid state reaction     CO2/H2    

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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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visible-photocatalytic hydrogen evolution and simultaneous organic pollutant degradation over an urchin-like oxygen-doped

《环境科学与工程前沿（英文）》 2022年 第16卷 第10期 doi: 10.1007/s11783-022-1566-z

摘要：

● An urchin-like OMS/ZIS composite was fabricated by a facile solvothermal method.

关键词： Dual-functional photocatalysts     Oxygen-doped MoS2/ZnIn2S4     H2 evolution     Organic pollutant    

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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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>In situ growth of phosphorized ZIF-67-derived amorphous CoP/Cu2O@CF electrocatalyst

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1430-1439 doi: 10.1007/s11705-023-2320-1

摘要： Transition metal phosphides have been extensively studied for catalytic applications in water splitting. Herein, we report an in situ phosphorization of zeolitic imidazole frameworks (ZIF-67) to generate amorphous cobalt phosphide/ZIF-67 heterojunction on a self-supporting copper foam (CF) substrate with excellent performance for hydrogen evolution reaction (HER). The needle-leaf like copper hydroxide was anchored on CF surface, which acted as implantation to grow ZIF-67. The intermediate product was phosphorized to obtain final electrocatalyst (CoP/Cu2O@CF) with uniform particle size, exhibiting a rhombic dodecahedron structure with wrinkles on the surface. The electrochemical measurement proved that CoP/Cu2O@CF catalyst exhibited excellent HER activity and long-term stability in 1.0 mol·L–1 KOH solution. The overpotential was only 62 mV with the Tafel slope of 83 mV·dec–1 at a current density of 10 mA·cm–2, with a large electrochemical active surface area. It also showed competitive performance at large current which indicated the potential application to industrial water electrolysis to produce hydrogen. First-principle calculations illustrated that benefit from the construction of CoP/ZIF-67 heterojunction, the d-band center of CoP downshifted after bonding with ZIF-67 and the Gibbs free energy (ΔGH*) changed from –0.18 to –0.11 eV, confirming both decrease in overpotential and excellent HER activity. This work illustrates the efficient HER activity of CoP/Cu2O@CF catalyst, which will act as a potential candidate for precious metal electrocatalysts.

关键词： CoP/Cu2O@CF     electrocatalyst     phosphorization     HER     DFT    

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Bamboo-like -doped carbon nanotubes encapsulating M(Co, Fe)-Ni alloy for electrochemical production of

《化学科学与工程前沿（英文）》 2022年 第16卷 第4期   页码 498-510 doi: 10.1007/s11705-021-2082-6

摘要： The electrochemical conversion of CO2-H2O into CO-H2 using renewable energy is a promising technique for clean syngas production. Low-cost electrocatalysts to produce tunable syngas with a potential-independent CO/H2 ratio are highly desired. Herein, a series of N-doped carbon nanotubes encapsulating binary alloy nanoparticles (MxNi-NCNT, M= Fe, Co) were successfully fabricated through the co-pyrolysis of melamine and metal precursors. The MxNi-NCNT samples exhibited bamboo-like nanotubular structures with a large specific surface area and high degree of graphitization. Their electrocatalytic performance for syngas production can be tuned by changing the alloy compositions and modifying the electronic structure of the carbon nanotube through the encapsulated metal nanoparticles. Consequently, syngas with a wide range of CO/H2 ratios, from 0.5:1 to 3.4:1, can be produced on MxNi-NCNT. More importantly, stable CO/H2 ratios of 2:1 and 1.5:1, corresponding to the ratio to produce biofuels by syngas fermentation, could be realized on Co1Ni-NCNT and Co2Ni-NCNT, respectively, over a potential window of –0.8 to –1.2 V versus the reversible hydrogen electrode. Our work provides an approach to develop low-cost and potential-independent electrocatalysts to effectively produce syngas with an adjustable CO/H2 ratio from electrochemical CO2 reduction.

关键词： electrochemical reduction of CO2     syngas     N-doped carbon nanotubes     encapsulated alloy nanoparticles     CO/H2 ratio    

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标题 作者 时间 类型 操作

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

Enhanced heterogeneous Fenton-like activity by Cu-doped BiFeO

Jie Mao, Xie Quan, Jing Wang, Cong Gao, Shuo Chen, Hongtao Yu, Yaobin Zhang

期刊论文

Cu-doped Bi/Bi2WO6 catalysts for efficient N2 fixation by photocatalysis

期刊论文

Hydrothermal synthesis of crystalline α-/β-MnO2 nanorods via γ-MnOOH nanorod precursors

ZHANG Weixin, REN Xiangbin, YANG Zeheng, WANG Hua, WANG Qiang, HUANG Fei

期刊论文

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

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

Atomic force microscopy study on the microtopography of natural organic matter and newly formed hydrous MnO2

GUO Jin, MA Jun, SHI Xuehua

期刊论文

Preparation and investigation of Pd doped Cu catalysts for selective hydrogenation of acetylene

Xinxiang Cao, Tengteng Lyu, Wentao Xie, Arash Mirjalili, Adelaide Bradicich, Ricky Huitema, Ben W.-L. Jang, Jong K. Keum, Karren More, Changjun Liu, Xiaoliang Yan

期刊论文

Preparation of Cu/ZrO

Xinmei LIU, Shaofen BAI, Huidong ZHUANG, Zifeng YAN

期刊论文

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

visible-photocatalytic hydrogen evolution and simultaneous organic pollutant degradation over an urchin-like oxygen-doped

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

>In situ growth of phosphorized ZIF-67-derived amorphous CoP/Cu2O@CF electrocatalyst

期刊论文

Bamboo-like -doped carbon nanotubes encapsulating M(Co, Fe)-Ni alloy for electrochemical production of

期刊论文