Science China-Materials
·
2021
·Vol. 65
·期 3
·721-731
·
IF 8.273
Xu Hui,Jin Meng,Geng Jing,Zhang Shengbo,Zhang Haimin
The decentralized production of H 2 O 2 via a two-electron oxygen reduction reaction (2e − ORR) has emerged as a promising alternative to the energy-intensive anthraquinone (AQ) process. However, its practical application requires 2e − ORR electrocatalysts with high activity and selectivity. Herein, we report the synthesis of metallic Ni nanoparticles anchored on bacterial cellulose-derived carbon fibers (Ni-NPs/BCCF) via a facile impregnation-pyrolysis method as efficient electrocatalysts for 2e − ORR to H 2 O 2 . By tuning the amount of Ni precursor, the best electrocatalytic performance toward 2e − ORR was achieved for Ni-NPs/BCCF-20.7, affording a high H 2 O 2 selectivity of ∼90% and an onset potential of 0.75 V vs. reversible hydrogen electrode (RHE) in an alkaline electrolyte. Ni-NPs/BCCF-20.7 achieved the largest H 2 O 2 yield rate of 162.7 ± 13.7 mmol g cat −1 h −1 and the highest Faradaic efficiency of 93.9% ± 4.2% at 0.2 and 0.5 V vs. RHE from the bulk ORR system, respectively. Theoretical calculations revealed the more favorable “end-on” adsorption configuration of molecular oxygen on the exposed Ni(111) plane, which can effectively suppress the O-O bond dissociation, resulting in high selectivity for H 2 O 2 generation.
研究领域:
材料化学
·
电化学
·
纳米催化
·
能源科学
·
环境工程
✓ 已验证
DOI
高影响因子
ChemSusChem
·
2019
·Vol. 12
·期 4
·858-865
·
IF 7.804
Xinxin Li,Qingshan Zhao,Xiang Feng,Lei Pan,Zhuangzhuang Wu,Xiaocui Wu,Tianwen Ma,Jialiang Liu,Yuanyuan Pan,Yan Song,Mingbo Wu
Graphical Nitrogen-doped graphene nanoshells supporting palladium nanoparticles (Pd/N-GNS) have been developed as a superior catalyst for the N -allylation reaction. Experimental results and DFT calculations reveal strong metal–support interactions between the pyridinic N and palladium species, which significantly boost the catalytic efficiency and stability of the catalyst. In this study, nitrogen-doped graphene nanoshells (N-GNS) were developed to support palladium nanoparticles (Pd/N-GNS) as an efficient and recyclable catalyst for the N -allylation reaction. N-GNS was synthesized through a facile hard-template method by using petroleum asphalt, followed by nitrogen doping by thermal annealing with urea, the contents and species of which could be altered by the calcination temperature. Palladium nanoparticles (Pd NPs) with an average diameter of 3.3 nm were homogeneously deposited onto the N-GNS support through a mild solvent-growth approach. The Pd/N-GNS exhibited a superior activity towards the N -allylation reaction, 6-fold higher than that of the pristine graphene nanoshells supporting the palladium catalyst. The Pd/N-GNS could be recycled several times without activity deterioration and metal leaching. The catalytic activity showed a linear correlation relationship with the pyridinic N content. Experimental and theoretical studies reveal strong metal–support interactions between the pyridinic N and palladium species, which can downsize the Pd NPs, modulate the electronic properties, and promote the adsorption of reactant, thereby significantly boosting the catalytic efficiency and stability for the N -allylation process. The present work could help unravel the roles of nitrogen-doped carbon supports and provides a feasible strategy to rationally design superior palladium catalysts for chemical transformations.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Xijun Wei,Yanhong Li,Huarong Peng,Ming Zhou,Yingqing Ou,Yibin Yang,Yunhuai Zhang,Peng Xiao
In this work, hollow CoS nanobox (noted as HCSN) have been successfully synthesized via annealing and hydrothermal process from zeolitic imidazolate framework (ZIF-67) template. When tested as positive electrode materials in alkaline aqueous electrolyte, it shows high specific capacitance of 720 F g −1 at a current density of 1 A g −1 , good rate capability (82.1%) and good cycling stability with 86.4% capacitance retention over 10,000 cycles at 10 A g −1 . To further demonstrate the advantages of our ZIF-67 derived materials, asymmetric energy storage device was assembled (HCSN//NC), where the as-prepared HCSN was employed as the anode and ZIF-67-derived nanoporous carbon (noted as NC) as the cathode. This device achieves high energy density (80 Wh kg −1 at a specific power density of 882 W kg −1 ), good rate capability (53.3 Wh kg −1 even at a specific power density of 7.9 kW kg −1 ) and long-term stability up to 10,000 cycles. More importantly, it could simultaneously light up 12 LEDs in parallel, demonstrating its potential in practical applications.
研究领域:
材料科学
·
电化学
·
纳米科技
·
能源存储
·
功能材料
·
应用物理
✓ 已验证
DOI
高影响因子
JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
·
2018
·
IF 2.207
Hongyu Shi,Na Li,Zhixia Sun,Tianqi Wang,Lin Xu
TiO 2 nanoparticles are commonly used as versatile precursors to make functional nanocomposite materials. However, the surface defects at grain boundaries of TiO 2 nanoparticles significantly affect the photoelectric properties of TiO 2 nanomaterials . In this work, we firstly prepared nanocomposites of TiO 2 and polyoxometalates (POMs) in which different POMs, including titanium-substituted POMs K 5 [PW 11 TiO 40 ] and K 7 [PW 10 Ti 2 O 40 ], are incorporated with TiO 2 nanoparticles so as to make an interface modification on grain boundaries of TiO 2 nanoparticles. Then the photoconductivities of the TiO 2 /POM nanocomposites were investigated through measurement of photocurrent responses, current-voltage curves, Mott-Schottky plots and surface photocurrent spectra. Compared with pure TiO 2 nanoparticles, TiO 2 /POM nanocomposites exhibit superior photoelectric properties, benefitting from the interface modification from different POMs. The gas sensing performance for acetone was also explored by use of the as-prepared photoconductive devices, and TiO 2 /PW 11 Ti exhibited a high gas sensing performance.
研究领域:
材料科学
·
纳米科技
·
半导体物理
·
传感器技术
·
光电子学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2013
·Vol. 38
·期 25
·10932-10938
·
IF 3.548
H. Wang,J. Zhang,J.W. Liu,L.Z. Ouyang,M. Zhu
In this study, alkali hydroxides (NaOH, LiOH, KOH) were attempted as new-type catalytic additives to improve the hydrogen storage properties of MgH 2 by ball milling . It is shown that the additives readily react with the MgH 2 to form perovskite-structured NaMgH 3 and KMgH 3 , but not the LiMgH 3 . Although the in-situ formed perovskite hydrides remain stable during hydriding/dehydriding cycles, both NaMgH 3 and KMgH 3 show predominant catalytic role on the hydriding and dehydriding of MgH 2 . In contrast, the LiOH modified MgH 2 presents much inferior sorption kinetics because of the absence of LiMgH 3 . The catalytic mechanism of perovskite hydrides can be explained by the high hydrogen mobility in the perovskite structure . This study shows that such cheap hydroxides could be used as efficient catalysts to improve the hydrogen storage properties of high-capacity metal hydrides and complex hydrides .
研究领域:
材料科学
·
无机化学
·
能源化学
·
氢能存储
·
金属氢化物
·
固态储氢
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2017
·Vol. 52
·期 19
·11701-11714
·
IF 2.599
Wei Xiuzhen,Hong Jialiang,Zhu Shuangshuang,Chen Jinyuan,Lv Bosheng
Polyethyleneimine (PEI) of various molecular weights and trimesoyl chloride (TMC) were utilized to prepare composite nanofiltration (NF) membranes via interfacial polymerization. The changes in the surface structure and chemical composition of the prepared membranes were evaluated using SEM, ATR-FTIR, XPS and surface potential measurements. The pure-water flux and rejection rates of the inorganic salts (MgCl 2 , MgSO 4 , Na 2 SO 4 and NaCl) through the resultant NF membranes were also investigated. The results showed that the performance of the composite NF membranes was significantly affected by the molecular weight of the PEI. Notably, the permeate flux and rejection rate of the NF membranes increased with the PEI molecular weight. In addition, when the NF membranes were used to treat actual wastewater from the electroplating industry, the NF membranes presented high-efficiency separation properties for heavy metal ions. The rejection rates of the NF membranes at 0.4 MPa for chromium, nickel, zinc and copper ions reached 92.6, 89.6, 89.2 and 86.3%, respectively.
研究领域:
材料科学
·
膜分离技术
·
环境工程
·
高分子化学
·
水处理
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 36
·19536-19545
·
IF 11.9
Gege Wang,Feifan Zhang,Caiyu Ma,Jianhua Yang,Xiaowei Chi,Yu Liu
Aqueous zinc metal batteries (AZMBs) as one of the next-generation energy storage technologies have attracted both academic and industrial attention due to their high safety, low cost, and high specific energy, yet are facing interfacial challenges at the electrolyte/anode interface, e.g. uneven physical diffusion of Zn2+ flux, severe chemical corrosion, and disordered electrochemical deposition behavior of the zinc metal anode. To address these issues, herein, we propose a facile and effective electrolyte modulating strategy to construct a physico-chemo-electrochemically coupled stable interface between the aqueous electrolyte and zinc anode. The aqueous electrolyte modified using a tiny amount of water-soluble ionic liquid 1-ethyl-3-methylimidazolium tetrafluoroborate (EMIMBF4) can form a positively charged organic EMIM+ adsorption layer and a protective inorganic Zn2+-conducting layer through the in situ decomposition of BF4− on the zinc anode surface, thus effectively homogenizing the Zn2+ diffusion flux and decreasing the chemical corrosion rate. Moreover, EMIM+ provides an electrostatic shielding layer, leading to the preferential and ordered electrodeposition of Zn2+ along the Zn (002). Benefiting from this physico-chemo-electrochemically multifunctional interfacial layer, the Zn//Zn symmetric cells achieve a considerably extended lifespan of up to 1200 h at 5 mA cm−2 and 5 mA h cm−2, and more than 450 h even at an ultrahigh current density and large deposition capacity (10 mA cm−2 and 10 mA h cm−2). Zn//Cu asymmetric cells also exhibit excellent reversibility with a high coulombic efficiency of 99.75%. Furthermore, the physically, chemically, and electrochemically stabilized interface enables the AZMB with a quinone-based cathode to offer high specific capacity (256.9 mA h g−1) and a decent capacity retention rate (83.9% after 300 cycles).
研究领域:
电化学
·
能源材料
·
界面科学
·
储能技术
·
材料化学
✓ 已验证
DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2022
·
IF 3.428
Baoqin Mu,Bin Li,Bin Qi
Lanthanide metal–organic framework Ln-MOFs(Ln = Sm, Dy, Dy/Sm) were synthesized by hydrothermal method at 100 °C for 12 h using lanthanide metals (Ln = Sm, Dy, Dy/Sm) as metal ion centers and 1,3,5-benzotrioic acid (H 3 BTC) as ligands. The structural characteristics of Ln(BTC)(H 2 O)·(DMF) were characterized by X-ray Diffraction(XRD), Fourier Transform Infrared Spectroscopy(FT-IR) and Thermogravimetric Analysis(TGA). Scanning electron microscopy showed that the samples showed rod-like morphology, and the fluorescence spectra showed 478 nm and 573 nm corresponding to the characteristic transitions of 4 F 9/2 → 6 H 15/2 (blue light) and 4 F 9/2 → 6 H 13/2 (yellow light) of Dy 3+ , respectively, while orange light at 600 nm and red light at 646 nm corresponded to the characteristic transitions of 4 G 5/2 → 6 H 7/2 and 4 G 5/2 → 6 H 9/2 of Sm 3+ , demonstrating that the double-doped lanthanide metal ions MOF were successfully synthesized. H 7 (P(Mo 2 O 7 ) 6 )/(Dy/Sm-MOF) was used as a sensor for the determination of H 2 PO 4 − , the results of performance evaluation showed that the electrochemical sensor showed a linear relationship between 0.01 and 0.17 mM for H 2 PO 4 − , with a detection limit of 0.005 mM/L, good stability and reproducibility, which opened up a new way for the detection of orthophosphate dihydrogen.
研究领域:
分析化学
·
材料科学
·
电化学
·
无机化学
·
传感器技术
✓ 已验证
DOI
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 72
·45420-45431
·
IF 3.108
Jiuli Guo,Huanhuan Yu,Feng Dong,Baolin Zhu,Weiping Huang,Shoumin Zhang
A highly efficient and stable Au–Cu/hydroxyapatite (HAP, Ca10(PO4)6(OH)2) catalyst was reported. HAP was prepared through a deposition–precipitation method. Au–Cu/HAP catalysts were obtained by a two-step impregnation approach. The samples were characterized by XRD, TEM, SEM, UV-Vis, ICP, XPS, H2-TPR, and O2-TPD. CO oxidation reaction was carried out to evaluate the catalytic performance of samples. TEM and UV-Vis results showed that the metallic particles supported on Au–Cu/HAP were smaller than those on Au/HAP, and they were highly dispersed on the HAP support. Patterns of XPS revealed that CuO nanoparticles were formed in the Cu/HAP catalyst, while CuO and Cu2O species coexisted in Au–Cu/HAP catalyst. Based on the O2-TPD data, the addition of copper to Au/HAP gave rise to more new O2 adsorption sites and bigger O2 adsorption capacity. The catalysis results indicated that the Au–Cu/HAP was capable of obtaining higher efficiency and stability compared with Au/HAP and Cu/HAP for CO oxidation. It was likely that the synergistic interaction between gold and CuOx phase created the most active sites on Au–Cu/HAP and was responsible for the enhanced activity and stability in comparison with Au/HAP and Cu/HAP.
研究领域:
催化化学
·
材料科学
·
环境化学
·
纳米催化
·
表面科学
✓ 已验证
DOI
高影响因子
CRYSTENGCOMM
·
2014
·Vol. 16
·期 37
·8910-8916
·
IF 3.858
Feng Ye,Hui Liu,Wenlai Huang,Jun Yang
Controlling the morphology of noble metal nanoparticles can be an effective way to produce nanomaterials with favourable properties. Herein, we report our study on the effects of diffusion rate and reaction kinetics on the morphology of a number of noble metal (Au, Ag, Pd, and Pt) nanoparticles. A glass reactor based on electrochemical reduction or photo-reduction has been designed to achieve control of diffusion and chemical reduction of the different noble metal precursors. The results show that the noble metal nanoparticles with flower-like, core–shell, or wheel-like morphologies could be obtained at a relatively high diffusion rate due to the presence of additional growth of metal precursors on the preformed metal nuclei, while at relatively low diffusion, the as-prepared noble metal nanoparticles are small and quasi-spherical due to the relatively fast reduction of metal precursors. The experimental observations are also confirmed qualitatively by kinetic Monte Carlo (kMC) simulations. Since diffusion and reaction kinetics are universal and key factors in the synthesis of nanomaterials, the findings in this work might provide an effective way to manipulate the morphology of nanomaterials for a given application.
研究领域:
纳米材料科学
·
物理化学
·
材料合成
·
胶体与界面化学
·
计算材料学
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2020
·
IF 7.183
Yanwei Sun,Chunshan Song,Xinwen Guo,Sungwon Hong,Jungkyu Choi,Yi Liu
Metal-organic framework (MOF) membranes have received increasing attention due to their unprecedented potential for energy-efficient gas separation. Compared with other MOF materials (like ZIF), fabrication and microstructural manipulation of high-performance Ti-MOF-based membranes, although being very attractive due to their excellent chemical and thermal stability, remained relatively less investigated due to the limitations of available titanium sources and heating modes. In this study, different Ti sources (TPOT, TiS 2 , and MXene) and heating modes (conventional heating, multi-mode microwave heating, and single-mode microwave heating) were examined for the preparation of NH 2 -MIL-125 membranes showing diverse microstructures and gas separation performances. The present work revealed that for the first time, MXene , the new two-dimensional Ti carbide , could be used as Ti source for synthesizing MOF membranes. The best performing NH 2 -MIL-125 membranes, which were obtained with TiS 2 as the metal source under single-mode microwave heating, exhibited the highest H 2 /CO 2 selectivity (ca. 17.2) as well as considerable H 2 permeance (1.7 × 10 −7 mol m −2 s −1 Pa −1 ), owing to an enhanced non-thermal effect of single-mode microwave heating and balanced dissolution rate of TiS 2 .
研究领域:
材料科学
·
膜分离技术
·
化学工程
·
纳米材料
·
气体分离
·
可持续能源
✓ 已验证
DOI
高影响因子
Sustainable Energy & Fuels
·
2021
·Vol. 5
·期 5
·1538-1547
·
IF 6.367
Ruyan Lei,Yanping Yang,Chenjuan Yu,Yinsi Xu,Yuanzhuo Li,Jun Li
In order to improve the electrochemical performance and efficiently prepare a solid polymer electrolyte (SPE) for the lithium-metal battery (LMB), a fumed SiO2 (FS) with surface Si–OH group was used to fabricate FS-modified poly(ethylene oxide) (PEO)–LiClO4-based SPE by a facile preparation process. The influences of the FS content on the morphological properties, thermal properties, lithium salt dissociation, mechanical properties, and electrochemical properties of SPE were systematically analyzed. Results indicate that FS with the hydrophilic property was widely distributed throughout the amorphous phase of SPE, thus the crystallinity of SPE was reduced to 25.83% when the FS mass loading was 6.85 wt%. In addition, a greater dissociation degree of lithium salt was achieved after the addition of FS, and a higher ion conductivity of 3.03 × 10−4 S cm−1 and Li-ion migration number of 0.396 were recorded at 60 °C. The all-solid-state Li/SPE/Li coin cell showed excellent stable cyclability (380 h) and the LiFePO4 (LFP)/SPE/Li coin cell demonstrated good discharge specific capacity and coulomb efficiency of 96 mA h g−1 and 100.2%, respectively, after 100 cycles of galvanostatic charge–discharge operation under 0.5C at 60 °C. Thus, based on collective results, it is expected that SPE presented in this work is a promising electrolyte for next-generation high-energy all-solid-state LMB with enhanced safety.
研究领域:
材料科学
·
电化学
·
能源存储
·
高分子化学
·
固态离子学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）