CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Lin Li,Chao Feng,Haimei Xu,Ping He,Qisong Yi,Junxiang Jiang,Lu Lin,Jin Hou,Yuanshuai Liu
The catalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is an important reaction in the sustainable production of polymers from biomass resources. To advance the environmental sustainability of this process, it is crucial to develop a catalytic system that circumvents the need for liquid alkaline media, which have been conventionally employed in HMF-to-FDCA conversion. Herein, we developed an efficient catalytic system comprising Ru nanoparticles supported on Na-type zeolite Y (Ru/Na-Y) for the base-free oxidation of HMF to FDCA. Reducing the particle size of Ru significantly enhances the activity of the Ru/Na-Y catalysts. Specifically, the optimized Ru/Na-Y-300N-200H, featuring Ru nanoparticles with an average size of ∼2.5 nm, afforded nearly 100 % HMF conversion and ∼ 85 % FDCA yield under base-free aqueous-phase conditions at 100 °C and 5 MPa air pressure. Kinetic studies further evidenced that Ru/Na-Y-300N-200H could effectively catalyze the sequential oxidation of both alcohol and aldehyde groups during the HMF-to-FDCA conversion. Comprehensive characterizations and DFT calculations elucidated the enhanced interaction between Ru centers and Na sites in the Ru/Na-Y-300N-200H due to the smallest Ru particle size. The unique Ru-Na synergistic effect was thus realized, which could facilitate the activation of O 2 and the generation of O 2 •– radicals as active oxygen species, while simultaneously boosting the rate-determining step of 5-formyl-2-furancarboxylic acid (FFCA) oxidation to FDCA, resulting in a high FDCA yield. These findings unveil promising prospects for developing advanced metal-zeolite bifunctional catalysts, which could facilitate the base-free oxidation of biomass-derived HMF into FDCA.
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INTERNATIONAL JOURNAL OF PHOTOENERGY
·
2012
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IF 1.769
Quan Gu,Huaqiang Zhuang,Jinlin Long,Xiaohan An,Huan Lin,Huaxiang Lin,Xuxu Wang
The C-doped CdO photocatalysts were simply prepared by high-temperature solid-state process. The as-prepared photocatalysts were characterized by X-ray powder diffraction (XRD), diffuse reflectance spectroscopy (UV-Vis DRS), scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS). The results demonstrated that the carbon was doped into CdO, resulting in the red-shift of the optical absorption of CdO. The photocatalytic behavior of CdO and C-doped CdO was evaluated under the visible light irradiation by using the photocatalytic hydrogen evolution as a model reaction. The C-doped CdO photocatalysts had higher photocatalytic activity over parent CdO under visible light irradiation. The results indicated that the H2 production was due to the existence of CdS and the enhancement of visible light photocatalytic activity of H2 production was originated from the doping of carbon into the CdO lattice. The probably reaction mechanism was also discussed and proposed.
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ELECTROCHIMICA ACTA
·
2016
·
IF 4.803
Zhen Liu,Huajun Zhou,Simon S. Ang,Jian-Jun Zhang
Here we report the evaluation of natrochalcite (Na[Cu 2 (OH)(H 2 O)(SO 4 ) 2 ]), an anionic layered structure [Cu 2 (OH)(H 2 O)(SO 4 ) 2 ] − charge-balanced by Na + , as an anode material for both Li- and Na-ion batteries. It delivers 224 mAh/g and 175 mAh/g in the first discharge in the Li + - and Na + -cells respectively, and decomposes to form amorphous matrixes during this step. In the subsequent charge, the original layered structure is unusually partially recrystallized back from the matrixes, resulting in 53 mAh/g and 35 mAh/g discharge capacities in the second discharge respectively. In subsequent cycling, Li + in the electrolyte is found to replace the original Na + during cycling in the Li + -cell and the electrode in the Li + -cell demonstrates better capacity retention rates than that in the Na + -cell, possibly due to Li + being smaller than Na + and thus decomposition-recrystallization cycles being more reversible during cycling in the Li + -cell.
研究领域:
材料科学
·
电化学
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 32
·15762-15770
·
IF 9.931
Xi Cao,Lulu Wang,Jitao Chen,Junrong Zheng
A Mg2+/Na+ hybrid aqueous battery with high energy density and low cost is constructed using commercial Mn3O4 as a cathode and NaTi2(PO4)3 as an anode for the first time. During electrochemical cycling, spinel Mn3O4 experiences a transition to layered MnO2 hosting Mg2+/Na+ with a high specific capacity and a long cycling life in Mg2+/Na+ hybrid electrolytes. The battery delivers a discharge potential above 1.2 V and an energy density over 47 W h kg−1 (based on the total mass of electrode materials) at a power density of 48 W kg−1; even at a high power density of 400 W kg−1, it delivers an energy density of 23.6 W h kg−1. What is more, the battery shows an excellent cycling performance with 94% capacity retention after 6000 cycles at 10C. The performances drop only very slightly for batteries prepared by an economic and scalable method. The excellent electrochemical properties, combined with the low cost of raw materials and the ease of scaling up which many aqueous batteries lack, make this approach a very promising cost-effective environment-friendly solution for large-scale energy storage.
研究领域:
材料科学
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电化学
·
储能技术
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PHYSICAL REVIEW B
·
2026
·Vol. 114
·期 2
·L020504
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IF 3.9
Yingying Gao,W. Zhou,W. H. Guo,Chunqiang Xu,H. F. Chen,Z. D. Han,Xiaofeng Xu,Yinzhong Wu,B. Qian
The observation of $\mathrm{high}\text{\ensuremath{-}}{T}_{\mathrm{c}}$ superconductivity in bilayer nickelate ${\mathrm{La}}_{3}{\mathrm{Ni}}_{2}{\mathrm{O}}_{7}$ under high pressure provides a new venue for exploring novel unconventional superconductors and elucidating the mechanism of $\mathrm{high}\text{\ensuremath{-}}{T}_{\mathrm{c}}$ superconductivity. Subsequently, numerous chemical substitution studies have been reported, aiming to stabilize superconductivity at ambient pressure or significantly reduce the pressure threshold required for its occurrence. Here, we report the comprehensive study of sodium (Na) doping in the Ruddlesden-Popper nickelate ${\mathrm{La}}_{3}{\mathrm{Ni}}_{2}{\mathrm{O}}_{7+\ensuremath{\delta}}$, where $\mathrm{N}{\mathrm{a}}^{+}$ substitutes for $\mathrm{L}{\mathrm{a}}^{3+}$ at the A-site with varying doping concentrations $(x)$. The structural, thermal, magnetic, and electronic transport properties of as-synthesized polycrystalline samples were systematically investigated. X-ray diffraction analysis reveals that the dominant structure has changed from the 327 Amam phase to the 4310 Bmab phase when $x\ensuremath{\ge}0.075$, which is further corroborated by thermogravimetric analysis measurements. Substitution of $\mathrm{L}{\mathrm{a}}^{3+}$ with $\mathrm{N}{\mathrm{a}}^{+}$ within the 327 phase gives rise to a gradual expansion of the lattice. Meanwhile, resistivity measurements indicate that the resistivity anomaly associated with a density-wave-like (DW-like) transition is marginally suppressed and metallicity is significantly enhanced. Upon application of pressure, the DW-like transition can be further suppressed, whereas the low-T insulating behavior remains insensitive to pressure. These results offer critical insights into the roles of elemental substitution and charge carrier doping in steering the competing electronic phases in layered nickelates.
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Chemical Science
·
2024
·Vol. 15
·期 24
·9224-9239
·
IF 7.6
Yunan Qin,Seong-Gyu Choi,Lucia Mason,Jing Liu,Zongjian Li,Tao Gao
Sodium-ion batteries (SIBs) is a promising technology for next-generation energy storage. However, their performance is limited at low temperatures due to the inferior bulk and interfacial resistance of current electrolytes. Here we present a systematic study to evaluate carboxylate ester-based electrolytes for SIB applications, due to their favorable properties (i.e., low melting point, low viscosity and high dielectric constant). The effects of salt, concentration and solvent molecular structure were systematically examined and compared with those of carbonate-based electrolytes. By combining electrochemical tests with spectroscopic characterization, the performance of selective carboxylate ester-based electrolytes in hard carbon/Na and Na3V2(PO4)3/Na half-cells was evaluated. We found carboxylates enable high electrolyte conductivities, especially at low temperatures. However, carboxylates alone are inadequate to form a stable interphase due to their high reactivity, which can be addressed by choosing a suitable anion and facilitating anion-rich Na+ solvation by increasing salt concentration. Fundamental knowledge on the chemistry–property–performance correlation of this new family of electrolytes was obtained, and their benefits and pitfalls were thoroughly discussed. These discoveries and knowledge will shed light on the potential of carboxylate ester-based electrolytes and provide the foundation for further electrolyte engineering.
研究领域:
材料科学
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电化学
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JOURNAL OF MOLECULAR LIQUIDS
·
2020
·
IF 5.065
Zhenguo Dou,Ying Wang,Wenhui Fang,Chenglin Sun,Zhiwei Men
Raman spectra of acetonitrile (CH 3 CN)–sodium perchlorate (NaClO 4 ) mixture solutions at different concentrations and temperatures have been studied. It was suggested that the shifts and intensities of Raman modes of CH 3 CN varied significantly due a novel Fermi resonance (FR) was formed between the ν 2 ′ and ( ν 3 + ν 4 )′ bands of CH 3 CN-Na + complex. The phase transition underwent from the liquid to solid phase β at 223 K, and from β to α at 213 K, which were induced by the strong cationic-molecule interaction. In addition, the impact of Na + on FR was discussed by the FR parameters at different concentrations and temperatures.
研究领域:
物理化学
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分子光谱学
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Materials
·
2023
·Vol. 16
·期 8
·3184
·
IF 3.4
Yan Qian,Zeen Huang,Guantao Zhou,Chenan Chen,Yuhang Sang,Zuolong Yu,Legao Jiang,Yuning Mei,Yunxiao Wei
This study investigates the montmorillonite (MMT) content, rotational viscosity, and colloidal index of sodium montmorillonite (Na-MMT) as a function of the sodium agent dosage, reaction time, reaction temperature, and stirring time. Na-MMT was modified using different octadecyl trimethyl ammonium chloride (OTAC) dosages under optimal sodification conditions. The organically modified MMT products were characterized via infrared spectroscopy, X-ray diffraction, thermogravimetric analysis, and scanning electron microscopy. The results show that the Na-MMT with good properties (i.e., the maximum rotational viscosity and highest Na-MMT content with no decrease in the colloid index) was obtained at a 2.8% sodium carbonate dosage (measured based on the MMT mass), a temperature of 25 °C, and a reaction time of two hours. Upon organic modification of the optimized Na-MMT, OTAC entered the NA-MMT interlayer, and the contact angle was increased from 20.0° to 61.4°, the layer spacing was increased from 1.58 to 2.47 nm, and the thermal stability was conspicuously increased. Thus, MMT and Na-MMT were modified by the OTAC modifier.Keywords:montmorillonite;organic modification;characterization;property
研究领域:
材料科学
·
化学工程
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FUEL
·
2024
·
IF 6.7
Liangyong Chen,Rui Mao
Developing robust catalytic oxygen carriers (COC) to make Chemical-looping Oxidation Coupling of Methane (CL-OCM) economical and practical remains a big challenge. This work modified the Mn-based catalysts for co-feed OCM and tried to adapt them into CL-OCM process. COCs were specially designed with high faction of Mn-oxides to improve oxygen storage, with supports (pelletized from SiO 2 , MgO and TiO 2 ) of stable and porous structure to improve cyclic stability and to tune lattice oxygen reactivity, and with Na + dopant to improve conversion and selectivity. Among the COCs, Mn20Na2Si and Mn20Si (20 wt% Mn 2 O 3 supported on SiO 2 with/without 2.0 wt% Na 2 CO 3 dopants) exhibited excellent methane coupling activity. The averaged CH 4 conversion, C 2 selectivity and yield of Mn20Na2Si upon multiple redox cycles were 21.4 %, 79.6 % and 17.03 %, respectively. It showed improvements in C 2 selectivity and yield by 187 % and 163 % compared to Mn20Si. This work tried to establish the relationships between CL-OCM performance and lattice oxygen behaviors, since COC transports lattice oxygen to promote methane coupling as it performs as a catalyst during CL-OCM reduction. It is found that high C 2 -selectivity and CH 4 conversion are benefited from the constant oxygen transporting rate. Na + dopant improved the concentration of surface lattice oxygens, tuned the spatial arrangement of metal oxides, and stabilized the surface lattice oxygen in cyclic reactions. Due to Na + -doping, carbon deposition on Mn20Na2Si was avoided, and catalyst deactivation as well. Finally, a mechanism was developed to reveal how lattice oxygen species and their releasing rates affected surface reaction network, CH 4 conversion, C 2 selectivity and cyclic stability.
研究领域:
催化化学
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能源化学
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Engineering
·
2022
·
IF 12.834
Wenguang Wang,Yanqiu Zhang,Xiaobin Yang,Haixiang Sun,Yadong Wu,Lu Shao
Monovalent cation exchange membranes (M-CEMs) have been extensively applied in environmental remediation and energy harvesting such as the extraction of Na + or Li + from brine and seawater. However, owing to the limitations of membrane structures and materials, M-CEMs have a low perm-selectivity issue. Herein, we proposed a facile approach to construct a novel M-CEM with a Janus-charged structure, consisting of a positively-charged trimesic acid/polyethylenimine surface thin layer and a negatively charged commercial cation exchange membrane (CEM). Selectrodialysis results indicated that the Janus-charged M-CEMs could effectively suppress the migration of anions, which often occurred in porous CEMs, thereby enabling the novel Janus-charged M-CEMs to possess high perm-selectivity and high total cation fluxes. Compared with state-of-the-art M-CEMs, the Janus-charged M-CEM exhibited the highest perm-selectivity of 145.77 for Na + /Mg 2+ beyond the contemporary “Upper Bound” plot as well as the excellent perm-selectivity of 14.11 for Li + /Mg 2+ , indicating its great potentials in ion separation. This study can provide novel insights into the design of Janus-charged M-CEMs for ion separation in diverse environmental and energy applications.
研究领域:
环境科学
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能源材料
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膜技术
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Chinese Physics B
·
2022
·Vol. 31
·期 6
·068201
·
IF 1.652
Yuejun Ding,Feixiang Ding,Xiaohui Rong,Yaxiang Lu,Yong-Sheng Hu
Na-ion batteries (NIBs) are regarding as the optimum complement for Li-ion batteries along with the rapid development of stationary energy storage systems. In order to meet the commercial demands of cathodes for NIBs, O3-type Cu containing layered oxide Na0.90Cu0.22Fe0.30Mn0.48O2 with good comprehensive performance and low-cost element components is very promising for the practical use. However, only part of the Cu3+/Cu2+ redox couple participated in the redox reaction, thus impairing the specific capacity of the cathode materials. Herein, Mg2+-doped O3-Na0.90Mg0.08Cu0.22Fe0.30Mn0.40O2 layered oxide without Mn3+ was synthesized successfully, which exhibited improved reversible specific capacity of 118 mAh/g in the voltage range of 2.4–4.0 V at 0.2 C, corresponding to the intercalation/deintercalation of 0.47 Na+ (0.1 more than that of Na0.90Cu0.22Fe0.30Mn0.48O2). This work demonstrates an important strategy to obtain advanced layered oxide cathodes for NIBs.
研究领域:
电化学储能
·
材料科学
·
无机化学
·
能源材料
·
固态化学
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ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Zhiming Jia,Jianjun Li,Ziyu Jia,Haijing Wang,Jihong Wei,Zuqiang Sun,Renyun Kuang,Xu Han,Yaohua Liang,Haihui Chen,Gangyong Zhou,Guoping Liu
Sodium-ion batteries are considered one of the most promising energy storage systems for large-scale energy storage and low-speed electric vehicles. However, developing suitable anode materials with a high capacity and stable cycling performance for sodium-ion batteries remains a challenge. In this work, we report a layered ternary GeBi4Te7 anode material, which can be synthesized by a facile high-energy ball milling method. Its structure consists of GeBi2Te4 and Bi2Te3 layers stacked periodically along the c-axis, providing spacious two-dimensional channels for the rapid insertion and extraction of sodium ions. Electrochemical test results demonstrate that the prepared GeBi4Te7 anode exhibits a high reversible specific capacity of 449.4 mA h g–1 at a current density of 1 A g–1 and a high initial Coulombic efficiency of 96.4%. Moreover, the Na-reaction mechanism of GeBi4Te7 was investigated. The results indicate that GeBi4Te7 undergoes a multistep sodium ion storage process following the electrochemical sequence of its components. During the discharge, sodium ions inserted into the interlayer gaps of the layered structure first, and then Na2Te, NaBi, Na3Bi, and NaGe were generated sequentially. During the charging stage, GeBi4Te7 compounds can be regenerated after the sodium extraction. In addition, the GeBi4Te7 shows 90.8% capacity retention after 7400 cycles during the potential gap of 0–1.0 V. This research provides insights into exploring multimetal tellurides for applications in the field of energy storage.
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