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Activated carbon induced oxygen vacancies-engineered nickel ferrite with enhanced conductivity for supercapacitor

《化学科学与工程前沿(英文)》 2023年 第17卷 第12期   页码 2088-2100 doi: 10.1007/s11705-023-2352-6

摘要: Activated carbon induced oxygen vacancies-engineered nickel ferrite with enhanced conductivity for supercapacitor application

关键词: nickel ferrite conductivity     carbon oxygen vacancies    

Enhanced performance of oxygen vacancies on CO adsorption and activation over different phases of ZrO

《能源前沿(英文)》 2023年 第17卷 第4期   页码 545-554 doi: 10.1007/s11708-023-0867-7

摘要: The effect of oxygen vacancies on the adsorption and activation of CO2 on the surface of different phases of ZrO2 is investigated by density functional theory (DFT) calculations. The calculations show that the oxygen vacancies contribute greatly to both the adsorption and activation of CO2. The adsorption energy of CO2 on the c-ZrO2, t-ZrO2 and, m-ZrO2 surfaces is enhanced to 5, 4, and 3 folds with the help of oxygen vacancies, respectively. Moreover, the energy barrier of CO2 dissociation on the defective surfaces of c-ZrO2, t-ZrO2, and m-ZrO2 is reduced to 1/2, 1/4, and 1/5 of the perfect surface with the assistance of oxygen vacancies. Furthermore, the activation of CO2 on the ZrO2 surface where oxygen vacancies are present, and changes from an endothermic reaction to an exothermic reaction. This finding demonstrates that the presence of oxygen vacancies promotes the activation of CO2 both kinetically and thermodynamically. These results could provide guidance for the high-efficient utilization of CO2 at an atomic scale.

关键词: CO2 activation     oxygen vacancies     ZrO2     different phases    

Photoreduction adjusted surface oxygen vacancy of BiMoO for boosting photocatalytic redox performance

《化学科学与工程前沿(英文)》 2023年 第17卷 第12期   页码 1937-1948 doi: 10.1007/s11705-023-2353-5

摘要: In this study, Bi2MoO6 with adjustable rich oxygen vacancies was prepared by a novel and simple solvothermal-photoreduction method which might be suitable for a large-scale production. The experiment results show that Bi2MoO6 with rich oxygen vacancies is an excellent photocatalyst. The photocatalytic ability of BMO-10 is 0.3 and 3.5 times higher than that of the pristine Bi2MoO6 for Rhodamine B degradation and Cr(VI) reduction, respectively. The results display that the band energy of the samples with oxygen vacancies was narrowed and the light absorption was broadened. Meanwhile, the efficiency of photogenerated electron-holes was increased and the separation and transfer speed of photogenerated carriers were improved. Therefore, this work provides a convenient and efficient method to prepare potential adjustable oxygen vacancy based photocatalysts to eliminate the pollution of dyes and Cr(VI) in water.

关键词: Bi2MoO6     oxygen vacancies     photoreduction     Cr(VI)     RhB    

Enhanced photocatalytic water splitting with surface defective SrTiO

Junying LIU, Zhidong WEI, Wenfeng SHANGGUAN

《能源前沿(英文)》 2021年 第15卷 第1期   页码 700-709 doi: 10.1007/s11708-021-0735-2

摘要: Surface reconstructed SrTiO nanocrystals were synthesized by a thermal treatment process in presence of NaBH and SrTiO nanocrystals. The surface reconstruction of SrTiO nanocrystals is attributed to the introduction of surface oxygen vacancies or Ti sites (such as Ti and Ti ) during the hydrogenation treatment process. The light absorption and the charge transfer ability of SrTiO nanocrystals are simultaneously enhanced due to surface oxygen vacancies or Ti sites (such as Ti and Ti ), which are beneficial to photocatalytic water splitting. Meanwhile, these defects also change the redox potential of the photocatalysts. Since there existed a synergistic effect between the three, the ratio of hydrogen to oxygen production was also regulated.

关键词: SrTiO3     surface reconstruction     oxygen vacancies     photocatalytic water splitting    

Oxygen-deficient MoO/NiS heterostructure grown on nickel foam as efficient and durable self-supported

《化学科学与工程前沿(英文)》 2023年 第17卷 第4期   页码 437-448 doi: 10.1007/s11705-022-2228-1

摘要: High-performance and ultra-durable electrocatalysts are vital for hydrogen evolution reaction (HER) during water splitting. Herein, by one-pot solvothermal method, MoOx/Ni3S2 spheres comprising Ni3S2 nanoparticles inside and oxygen-deficient amorphous MoOx outside in situ grow on Ni foam (NF), to assembly the heterostructure composites of MoOx/Ni3S2/NF. By adjusting volume ratio of the solvents of ethanol to water, the optimized MoOx/Ni3S2/NF-11 exhibits the best HER performance, requiring an extremely low overpotential of 76 mV to achieve the current density of 10 mA∙cm‒2 (η10 = 76 mV) and an ultra-small Tafel slope of 46 mV∙dec‒1 in 0.5 mol∙L‒1 H2SO4. More importantly, the catalyst shows prominent high catalytic stability for HER (> 100 h). The acid-resistant MoOx wraps the inside Ni3S2/NF to ensure the high stability of the catalyst under acidic conditions. Density functional theory calculations confirm that the existing oxygen vacancy and MoOx/Ni3S2 heterostructure are both beneficial to the reduced Gibbs free energy of hydrogen adsorption (|∆GH*|) over Mo sites, which act as main active sites. The heterostructure effectively decreases the formation energy of O vacancy, leading to surface reconstruction of the catalyst, further improving HER performance. The MoOx/Ni3S2/NF is promising to serve as a highly effective and durable electrocatalyst toward HER.

关键词: molybdenum oxides     oxygen vacancies     heterostructure     electrocatalysts     hydrogen evolution reaction    

Cooperative effect between copper species and oxygen vacancy in CeZrCuO catalysts for carbon monoxide

《化学科学与工程前沿(英文)》 2021年 第15卷 第6期   页码 1524-1536 doi: 10.1007/s11705-021-2106-2

摘要: The effects of Zr doping on the existence of Cu and the catalytic performance of Ce0.7−xZrxCu0.3O2 for CO oxidation were investigated. The characterization results showed that all samples have a cubic structure, and a small amount of Zr doping facilitates Cu2+ ions entering the CeO2 lattice, but excessive Zr doping leads to the formation of surface CuO crystals again. Thus, the number of oxygen vacancies caused by the Cu2+ entering the lattice (e.g., Cu2+–□–Ce4+; □: oxygen vacancy), and the amount of reducible copper species caused by CuO crystals, varies with the Zr doping. Catalytic CO oxidation tests indicated that the oxygen vacancy and the reducible copper species were the adsorption and activation sites of O2 and CO, respectively, and the cooperative effects between them accounted for the high CO oxidation activity. Thus, the samples x = 0.1 and 0.3, which possessed the most oxygen vacancy or reducible copper species, showed the best activity for CO oxidation, with full CO conversion obtained at 110 °C. The catalyst is also stable and has good resistance to water during the reaction.

关键词: Ce–Zr–Cu–O     CO oxidation     reducible copper species     oxygen vacancy     cooperative effect    

Metal-free, carbon-based catalysts for oxygen reduction reactions

Zhiyi Wu,Zafar Iqbal,Xianqin Wang

《化学科学与工程前沿(英文)》 2015年 第9卷 第3期   页码 280-294 doi: 10.1007/s11705-015-1524-4

摘要: Developing metal-free, carbon-based catalysts to replace platinum-based catalysts for oxygen reduction reactions (ORRs) is an emerging area of research. In recent years, different carbon structures including carbon doped with IIIA-VIIA heteroatoms (C−M site-based, where M represents the doped heteroatom) and polynitrogen (PN) compounds encapsulated in carbon nanotubes (CNTs) (N−N site-based) have been synthesized. Compared to metallic catalysts, these materials are highly active, stable, inexpensive, and environmentally friendly. This review discusses the development of these materials, their ORR performances and the mechanisms for how the incorporation of heteroatoms enhances the ORR activity. Strategies for tailoring the structures of the carbon substrates to improve ORR performance are also discussed. Future studies in this area will need to include optimizing synthetic strategies to control the type, amount and distribution of the incorporated heteroatoms, as well as better understanding the ORR mechanisms in these catalysts.

关键词: oxygen reduction reaction     electrocatalysis     metal-free     carbon-based     polynitrogen    

“Charging” the cigarette butt: heteroatomic porous carbon nanosheets with edge-induced topological defectsfor enhanced oxygen evolution performance

《化学科学与工程前沿(英文)》 2023年 第17卷 第11期   页码 1755-1764 doi: 10.1007/s11705-023-2318-8

摘要: Owing to the complexity of electron transfer pathways, the sluggish oxygen evolution reaction process is defined as the bottleneck for the practical application of Zn–air batteries. In this effort, metal nanoparticles (Co, Ni, Fe, etc.) encapsulated within nitrogen-doped carbon materials with abundant edge sites were synthesized by one-step pyrolysis treatment using cigarette butts as raw materials, which can drastically accelerate the overall rate of oxygen evolution reaction by facilitating the adsorption of oxygenated intermediates by the edge-induced topological defects. The prepared catalyst of nitrogen-doped carbon porous nanosheets loaded with Co nanoparticles (Co@NC-500) exhibits enhanced catalytic activity toward oxygen evolution reaction, with a low overpotential of 350 mV at the current density of 10 mA·cm–2. Furthermore, the Zn–air battery assembled with Co@NC-500 catalyst demonstrates a desirable performance affording an open-circuit potential of 1.336 V and power density of 33.6 mW·cm–2, indicating considerable practical application potential.

关键词: oxygen evolution reaction     porous carbon nanosheets     Co nanoparticles     edge-induced topological defects     Zn–air batteries    

Performance and kinetics of iron-based oxygen carriers reduced by carbon monoxide for chemical looping

Xiuning HUA,Wei WANG,Feng WANG

《环境科学与工程前沿(英文)》 2015年 第9卷 第6期   页码 1130-1138 doi: 10.1007/s11783-015-0821-y

摘要: Chemical looping combustion is a promising technology for energy conversion due to its low-carbon, high-efficiency, and environmental-friendly feature. A vital issue for CLC process is the development of oxygen carrier, since it must have sufficient reactivity. The mechanism and kinetics of CO reduction on iron-based oxygen carriers namely pure Fe O and Fe O supported by alumina (Fe O /Al O ) were investigated using thermo-gravimetric analysis. Fe O /Al O showed better reactivity over bare Fe O toward CO reduction. This was well supported by the observed higher rate constant for Fe O /Al O over pure Fe O with respective activation energy of 41.1±2.0 and 33.3±0.8 kJ·mol . The proposed models were compared via statistical approach comprising Akaike information criterion with correction coupled with F-test. The phase-boundary reaction and diffusion control models approximated to 95% confidence level along with scanning electron microscopy results; revealed the promising reduction reactions of pure Fe O and Fe O /Al O . The boosting recital of iron-based oxygen carrier support toward efficient chemical looping combustion could be explained accurately through the present study.

关键词: chemical looping combustion     iron-based oxygen carriers     reduction kinetics     carbon monoxide     statistics    

Phosphorus transformation under the influence of aluminum, organic carbon, and dissolved oxygen at the

Ouchen Cai, Yuanxiao Xiong, Haijun Yang, Jinyong Liu, Hui Wang

《环境科学与工程前沿(英文)》 2020年 第14卷 第3期 doi: 10.1007/s11783-020-1227-z

摘要: The three simulation factors caused various changes in both water and sediment. Responses to simulations differed with the reported natural lakes and wetlands. Al has dominant effects on sediment P release control among the three factors. Adding sediment Al can be effective and safe under the simulated conditions. Polyphosphates were not generated, while added phytate was rather stable. The effects of sediment aluminum (Al), organic carbon (OC), and dissolved oxygen (DO) on phosphorus (P) transformation, at the water-sediment interface of a eutrophic constructed lake, were investigated via a series of simulative experiments. The above three factors had various influences on dissolved P concentration, water pH, water and surface sediment appearance, and P fractions. Additions of Al had the greatest effect on suppressing P release, and the water pH remained alkaline in the water-sediment system under various OC and DO conditions. No dissolution of the added Al was detected. 31P-NMR characterization suggested that OC addition did not promote biological P uptake to polyphosphates under oxic conditions. The simulation result on the added phytate indicated the absence of phytate in the original lake sediment. As compared to the reported natural lakes and wetland, the water-sediment system of the constructed lake responded differently to some simulative conditions. Since Al, OC, and DO can be controlled with engineering methods, the results of this study provide insights for the practical site restorations.

关键词: Phosphorus     Sediment     Simulation     Dissolved oxygen     Organic carbon     Aluminum    

Metal phosphonate-derived cobalt/nickel phosphide@N-doped carbon hybrids as efficient bifunctional oxygen

《化学科学与工程前沿(英文)》 2022年 第16卷 第9期   页码 1367-1376 doi: 10.1007/s11705-022-2153-3

摘要: The exploration of efficient bifunctional electrocatalysts for oxygen reduction reaction and oxygen evolution reaction is pivotal for the development of rechargeable metal–air batteries. Transition metal phosphides are emerging as promising catalyst candidates because of their superb activity and low cost. Herein, a novel metal phosphonate-derived cobalt/nickel phosphide@N-doped carbon hybrid was developed by a carbothermal reduction of cobalt/nickel phosphonate hybrids with different Co/Ni molar ratios. The metal phosphonate derivation method achieved an intimately coupled interaction between metal phosphides and a heteroatom-doped carbon substrate. The resultant Co2P/Ni3P@NC-0.2 enables an impressive electrocatalytic oxygen reduction reaction activity, comparable with those of state-of-the-art Pt/C catalysts in terms of onset potential (0.88 V), 4e selectivity, methanol tolerance, and long-term durability. Moreover, remarkable oxygen evolution reaction activity was also observed in alkaline conditions. The high activity is ascribed to the N-doping, abundant accessible catalytic active sites, and the synergistic effect among the components. This work not only describes a high-efficiency electrocatalyst for both oxygen reduction reaction and oxygen evolution reaction, but also highlights the application of metal phosphonate hybrids in fabricating metal phosphides with tunable structures, which is of great significance in the energy conversion field.

关键词: metal phosphonate     cobalt/nickel phosphide     N-doped carbon     oxygen electrochemistry     Zn−air battery    

Floret-like Fe–N nanoparticle-embedded porous carbon superstructures from a Fe-covalent triazine polymerboosting oxygen electroreduction

《化学科学与工程前沿(英文)》 2023年 第17卷 第5期   页码 525-535 doi: 10.1007/s11705-022-2232-5

摘要: Fe–Nx nanoparticles-embedded porous carbons with a desirable superstructure have attracted immense attention as promising catalysts for electrochemical oxygen reduction reaction. Herein, we employed Fe-coordinated covalent triazine polymer for the fabrication of Fe–Nx nanoparticle-embedded porous carbon nanoflorets (Fe/N@CNFs) employing a hypersaline-confinement-conversion strategy. Presence of tailored N types within the covalent triazine polymer interwork in high proportions contributes to the generation of Fe/N coordination and subsequent Fe–Nx nanoparticles. Owing to the utilization of NaCl crystals, the resultant Fe/N@CNF-800 which was generated by pyrolysis at 800 °C showed nanoflower structure and large specific surface area, which remarkably suppressed the agglomeration of high catalytic active sites. As expect, the Fe/N@CNF-800 exhibited unexpected oxygen reduction reaction catalytic performance with an ultrahigh half-wave potential (0.89 V vs. reversible hydrogen electrode), a dominant 4e transfer approach and great cycle stability (> 92% after 100000 s). As a demonstration, the Fe/N-PCNF-800-assembled zinc–air battery delivered a high open circuit voltage of 1.51 V, a maximum peak power density of 164 mW·cm–2, as well as eminent rate performance, surpassing those of commercial Pt/C. This contribution offers a valuable avenue to exploit efficient metal nanoparticles-based carbon catalysts towards energy-related electrocatalytic reactions and beyond.

关键词: Fe–Nx nanoparticles     hypersaline-confinement conversion     floret-like carbon     covalent triazine polymers     oxygen reduction reaction    

Construction of defect-containing UiO-66/MoSe heterojunctions with superior photocatalytic performance for wastewater treatment and mechanism insight

《化学科学与工程前沿(英文)》 2023年 第17卷 第4期   页码 449-459 doi: 10.1007/s11705-022-2226-3

摘要: Metal–organic frameworks are recognized as promising multifunctional materials, especially metal–organic framework-based photocatalysts, which are considered to be ideal photocatalytic materials. Herein, a new type of UiO-66/MoSe2 composite was prepared using the solvothermal method. The optimum composite was selected by adjusting the mass ratio of UiO-66 and MoSe2. X-ray diffraction analysis showed that the mass ratio influenced the crystal plane exposure rate of the composite, which may have affected its photocatalytic performance. The composite is composed of ultra-thin flower-like MoSe2 that wrapped around cubic UiO-66, a structure that increases the abundance of active sites for reactions and is more conducive to the separation of carriers. The photocatalytic properties of the composite were evaluated by measuring the degradation rate of Rhodamine B and the catalyst’s ability to reduce Cr(VI)-containing wastewater under visible light irradiation. Rhodamine B was decolorized completely in 120 min, and most of the Cr(VI) was reduced within 150 min. The photochemical mechanism of the complex was studied in detail. The existence of Mo6+ and oxygen vacancies, in addition to the Z-type heterojunction promote the separation of electrons and holes, which enhances the photocatalytic effect.

关键词: UiO-66/MoSe2     photocatalysis     dye-containing wastewater     heavy metal wastewater     oxygen vacancies    

3D Network nanostructured NiCoP nanosheets supported on N-doped carbon coated Ni foam as a highly activebifunctional electrocatalyst for hydrogen and oxygen evolution reactions

Miaomiao Tong, Lei Wang, Peng Yu, Xu Liu, Honggang Fu

《化学科学与工程前沿(英文)》 2018年 第12卷 第3期   页码 417-424 doi: 10.1007/s11705-018-1711-1

摘要:

A highly active bi-functional electrocatalyst towards both hydrogen and oxygen evolution reactions is critical for the water splitting. Herein, a self-supported electrode composed of 3D network nanostructured NiCoP nanosheets grown on N-doped carbon coated Ni foam (NiCoP/NF@NC) has been synthesized by a hydrothermal route and a subsequent phosphorization process. As a bifunctional electrocatalyst, the NiCoP/NF@NC electrode needs overpotentials of 31.8 mV for hydrogen evolution reaction and 308.2 mV for oxygen evolution reaction to achieve the current density of 10 mA·cm2 in 1 mol·L1 KOH electrolyte. This is much better than the corresponding monometal catalysts of CoP/NF@NC and NiP/NF@NC owing to the synergistic effect. NiCoP/NF@NC also exhibits low Tafel slope, and excellent long-term stability, which are comparable to the commercial noble catalysts of Pt/C and RuO2.

关键词: bimetallic phosphides     N-doped carbon     self-support     hydrogen evolution     oxygen evolution    

Ultrafine Fe-modulated Ni nanoparticles embedded within nitrogen-doped carbon from Zr-MOFs-confined conversionfor efficient oxygen evolution reaction

《化学科学与工程前沿(英文)》 2022年 第16卷 第7期   页码 1114-1124 doi: 10.1007/s11705-021-2087-1

摘要: Improvement of the low-cost transition metal electrocatalyst used in sluggish oxygen evolution reaction is a significant but challenging problem. In this study, ultrafine Fe-modulated Ni nanoparticles embedded in a porous Ni-doped carbon matrix were produced by the pyrolysis of zirconium metal-organic-frameworks, in which 2,2′-bipyridine-5,5′-dicarboxylate operating as a ligand can coordinate with Ni2+ and Fe3+. This strategy allows formation of Fe-modulated Ni nanoparticles with a uniform dimension of about 2 nm which can be ascribed to the spatial blocking effect of ZrO2. This unique catalyst displays an efficient oxygen evolution reaction electrocatalytic activity with a low overpotential of 372 mV at 10 mA·cm–2 and a small Tafel slope of 84.4 mV·dec–1 in alkaline media. More importantly, it shows superior durability and structural stability after 43 h in a chronoamperometry test. Meanwhile, it shows excellent cycling stability during 4000 cyclic voltammetry cycles. This research offers a new insight into the construction of uniform nanoscale transition metals and their alloys as highly efficient and durable electrocatalysts.

关键词: metal-organic framework     pyrolysis     ultrafine     Fe-modulated Ni nanoparticles     oxygen evolution reaction    

标题 作者 时间 类型 操作

Activated carbon induced oxygen vacancies-engineered nickel ferrite with enhanced conductivity for supercapacitor

期刊论文

Enhanced performance of oxygen vacancies on CO adsorption and activation over different phases of ZrO

期刊论文

Photoreduction adjusted surface oxygen vacancy of BiMoO for boosting photocatalytic redox performance

期刊论文

Enhanced photocatalytic water splitting with surface defective SrTiO

Junying LIU, Zhidong WEI, Wenfeng SHANGGUAN

期刊论文

Oxygen-deficient MoO/NiS heterostructure grown on nickel foam as efficient and durable self-supported

期刊论文

Cooperative effect between copper species and oxygen vacancy in CeZrCuO catalysts for carbon monoxide

期刊论文

Metal-free, carbon-based catalysts for oxygen reduction reactions

Zhiyi Wu,Zafar Iqbal,Xianqin Wang

期刊论文

“Charging” the cigarette butt: heteroatomic porous carbon nanosheets with edge-induced topological defectsfor enhanced oxygen evolution performance

期刊论文

Performance and kinetics of iron-based oxygen carriers reduced by carbon monoxide for chemical looping

Xiuning HUA,Wei WANG,Feng WANG

期刊论文

Phosphorus transformation under the influence of aluminum, organic carbon, and dissolved oxygen at the

Ouchen Cai, Yuanxiao Xiong, Haijun Yang, Jinyong Liu, Hui Wang

期刊论文

Metal phosphonate-derived cobalt/nickel phosphide@N-doped carbon hybrids as efficient bifunctional oxygen

期刊论文

Floret-like Fe–N nanoparticle-embedded porous carbon superstructures from a Fe-covalent triazine polymerboosting oxygen electroreduction

期刊论文

Construction of defect-containing UiO-66/MoSe heterojunctions with superior photocatalytic performance for wastewater treatment and mechanism insight

期刊论文

3D Network nanostructured NiCoP nanosheets supported on N-doped carbon coated Ni foam as a highly activebifunctional electrocatalyst for hydrogen and oxygen evolution reactions

Miaomiao Tong, Lei Wang, Peng Yu, Xu Liu, Honggang Fu

期刊论文

Ultrafine Fe-modulated Ni nanoparticles embedded within nitrogen-doped carbon from Zr-MOFs-confined conversionfor efficient oxygen evolution reaction

期刊论文