CHINESE JOURNAL OF CHEMISTRY
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2023
·Vol. 42
·期 6
·617-622
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IF 5.4
Wei-Xing Chen,Yu-He Xu,Cui-Cui Wang,Lei Qiao,Zi-Yan Guo,Wen-Juan Tian,Zhong-Ming Sun
Comprehensive Summary Binary polyantimony clusters, namely [Cu 2 Sb 14 ] 4– and [Ag 2 Sb 14 ] 4– , containing coinage metals, were successfully synthesized and characterized, in which two homoatomic Sb 7 3– subunits are bridged by two coinage metals in η 4 : η 1 and η 1 : η 1 coordination modes, respectively. In [Cu 2 Sb 14 ] 4– , two bridging Cu ions and two Sb atoms form a planar rhombic unit, which was revealed to have antiaromatic properties by theoretical calculations. Further electron structure and bonding analysis confirmed the presence of delocalized bonds in the rhombic unit and the metallophilic interaction between two formal M + ions.
研究领域:
无机化学
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团簇化学
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结构化学
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理论化学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Jiarui Zhao,Zhen Wang,Hao Wang,Yan Li,Changqing Fang
With the rapid development of communication technology, it will lead to many electromagnetic wave (EMW) pollutions affecting the normal operation of precision instruments in industry. Then need smart electromagnetic interference (EMI) shielding material to protect the instrument from electromagnetic radiation . In this paper, multi-dimensional architectures yolk-shell-like VO 2 (M)/Ti 3 C 2 T x MXene (MXene) composite films (VM) were successfully prepared by hydrothermal treatment and electrostatic self-assembly. Yolk-shell-like VO 2 (M) microspheres were riveted onto few-layer MXene nanosheets as a smart EMI shielding material. Above 65 °C, the metal-insulator phase transition (MIT) of VO 2 (M) changes from the semiconductor state to the metallic state. VM composite films possess temperature controlled EMI shielding properties, which have not been reported before. When the thickness is 29.06 µm, the composite sample exhibits an EMI SE of 43.5 dB at 85 °C, which is 8 dB higher than room temperature . Besides, the few-layer structure and the unique yolk-shell-like structure of VM composite films exhibit excellent dielectric loss. The introduction of few-layer MXene nanosheets improves the EMI shielding performance of yolk-shell-like VO 2 (M) microspheres and achieves optimized impedance matching. Therefore, VM composite films are expected to provide new ideas for smart EMI shielding materials.
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Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Jiajie Wang,Bairen Yang,Zhuqiu Sun,Qingqing Shang,Junheng Zhang
This study aimed to investigate the performance of biotrickling filters (BTFs) in the microbial degradation of m -dichlorobenzene ( m -DCB) to construct an enhanced treatment of removing m -dichlorobenzene ( m -DCB) at different concentrations of rhamnolipids (RLs) and lanthanum (La 3+ ) or neodymium (Nd 3+ ) ions. We found a significantly enhanced removal of m -DCB when 110 mg/L of RLs and 0.2 mg/L La 3+ or 0.4 mg/L Nd 3+ ions were added. The addition of RLs and La 3+ or Nd 3+ ions increased the m -DCB average removal efficiency (101–110 days) by 19.7% and 22.7%, respectively, when the inlet m -DCB concentration was 800 mg/m 3 and the empty bed residence time (EBRT) was 60 s. Further, the mechanisms that strengthened the mass transfer were the decrease of contact angle, surface tension, and Henry’s constant after the addition of RLs and La 3+ or Nd 3+ ions in the nutrient solution; further, we noticed a significant increase in the dissolved oxygen levels. Improvements in the performance of BTFs were associated with enhanced microbial community and an increased abundance of functional genes. In conclusion, the addition of RLs and La 3+ or Nd 3+ ions can enhance the performance of BTFs in degrading m -DCB by improving mass transfer and microbial activity simultaneously.
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Nanomaterials
·
2023
·Vol. 13
·期 4
·660
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IF 5.3
Shuanghong Liu,Guan Huang,Jiefei Wang,Jianshuai Bao,Mengyue Wang,Yaqun Wei,Yong Zhong,Feng Bai
Surface plasmon resonance (SPR) photocatalysts have attracted considerable attention because of their strong absorption capacity of visible light and enhanced photogenic carrier separation efficiency. However, the separate production of metal nanoparticles (NPs) and semiconductors limits the photogenic charge transfer. As one of the most promising organic photocatalysts, porphyrin self-assemblies with a long-range ordered structure-enhance electron transfer. In this study, plasmonic noble metal-based porphyrin hexagonal submicrowires composites (M-HW) loaded with platinum (Pt), silver (Ag), gold (Au), and palladium (Pd) NPs were synthesized through a simple in situ photocatalytic method. Homogeneous and uniformly distributed metal particles on the M-HW composites enhanced the catalytic or chemical properties of the organic functional nanostructures. Under the same loading of metal NPs, the methyl orange photocatalytic degradation efficiency of Ag-HW [kAg-HW(0.043 min−1)] composite was three times higher than that of HW, followed by Pt-HW [kPt-HW(0.0417 min−1)], Au-HW [kAu-HW(0.0312 min−1)], and Pd-HW [kPd-HW(0.0198 min−1)]. However, the rhodamine B (RhB) and eosin B photocatalytic degradations of Pt-HW were 4 times and 2.6 times those of HW, respectively. Finally, the SPR-induced electron injection, trapping, and recombination processes of the M-HW system were investigated. These results showed that M-HW plasmonic photocatalysts exhibited excellent photocatalytic performances, making them promising materials for photodegrading organic pollutants.Keywords:porphyrin;self-assemblies;surface plasmon resonance;photocatalytic
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Wen-Jian Yang,Li-Hui Yang,Han-Jun Peng,Si-Hao Lv,Hafiz Muhammad Adeel Sharif,Wei Sun,Wei Li,Cao Yang,Hui Lin
Electroreduction removal of nitrate (NO 3 – -N) is considered as a promising approach to solve its adverse effects on environment and human health, where efficient and cheap catalysts are required. Perovskite-based catalysts showed a versatile catalytic ability for wide range of redox reactions, but seldom applied for NO 3 – -N reduction. Herein, four perovskite oxide cathodes, LaMO 3-δ (M = Fe, Co, Ni and Cu) were prepared and used for the reduction of NO 3 – -N. The Ruddlesden-Popper (RP) type La 2 CuO 4 exhibited the best NO 3 – -N catalytic activity among the four perovskite oxide cathodes, with a removal rate of 11.7 × 10 -3 min −1 . The high selectivity of NH 4 + -N (82.4 ± 2.2%) indicated that NH 4 + -N was the main final product for NO 3 – -N electroreduction at La 2 CuO 4 cathode, but 100% of N 2 selectivity could be obtained with addition of 1000 and 1500 mg/L Cl - as the electro-assisted chlorination process. The mechanism of NO 3 – -N electroreduction occurred by both electron- and H*-mediated pathway, and the oxygen vacancies and redox cycle of Cu(I)-Cu(II)-Cu(I) were proposed as the accommodation sties and direct electron sources for NO 3 – -N reduction. Generally, this study opens a novel avenue for the development of earth-abundant, cost-effective catalyst with effective NO 3 – -N electroreduction.
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Small Structures
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2022
·Vol. 4
·期 1
·2200161
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IF 11.343
Lu Chen,Youbing Li,Ke Chen,Xiaojing Bai,Mian Li,Shiyu Du,Zhifang Chai,Qing Huang
Entropy stabilization is an effective method to design and explore MAX phases with outstanding properties via tuning constituent elements and crystal structures, which have received considerable critical attention. Currently, some medium-/high-entropy (ME/HE) MAX phases, whose A layers are composed of Al, S, and magnetic elements, are reported, while few discussions about ME/HE-MAX phases with other A elements (e.g., Sn) are conducted. Herein, fully dense ME/HE-MAX phase bulks ((TiVNb) 2 SnC, (TiVNbZr) 2 SnC, and (TiVNbZrHf) 2 SnC) are designed and synthesized because of the chemical diversity of MAX phases. The results of Rietveld refinement of X-ray diffraction, scanning electron microscopy, and high-resolution scanning transmission electron microscopy-affiliated energy-dispersive spectrometer analysis comprehensively verify the crystal structure of ME/HE-MAX phases. Both the electrical conductivity and the charge carrier mobility are significantly lower than the reported correlation ternary MAX phases, due to the electron scattering and structural defects in ME/HE-MAX phase crystal structures. Similarly, the electron contribution of thermal conductivity is gradually declining; on the contrary, the phonon plays an increasingly dominant role as temperature increases. Owing to the richness in composition of MAX phases, herein, a composition design route for discovering new MAX phases and tuning their properties is indicated.
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JOURNAL OF CATALYSIS
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2022
·
IF 8.047
Beilei Cui,Hua Wang,Jinyu Han,Qingfeng Ge,Xinli Zhu
The relatively cheap and abundant Ni as a catalyst for hydrodeoxygenation (HDO) of biomass lignin-derived phenolics at 350 °C and atmospheric pressure suffers from unfavorable C-C hydrogenolysis toward CH 4 with a lower direct deoxygenation (DDO) activity. Herein, we demonstrate that the activity and selectively of Ni for HDO of m-cresol can be modified through the differences of strong metal-support interaction (SMSI) on anatase and rutile TiO 2 . Characterizations showed that the presence of SMSI depended strongly on the crystal phase of TiO 2 . The SMSI dominates on Ni/a-TiO 2 after reduction at 350 °C, resulting in Ni particles partially covered by a TiO x overlayer, and this overlayer became sufficiently thick at 650 °C, causing a significant reduction of CO chemisorption. Although the catalyst became selective for DDO to toluene, the overall HDO activity was significantly reduced because of excessive SMSI. In contrast, the Ni/r-TiO 2 catalyst reduced at 350 °C exhibited little SMSI and was active for C-C hydrogenolysis like a bare Ni catalyst. Increasing reduction temperature to 650 °C, the Ni/r-TiO 2 catalyst showed moderate SMSI and became selective to toluene through DDO while completely inhibited CH 4 formation. The toluene and total aromatics yields were 84.8 and 92.2%, respectively, at full conversion. More importantly, the turnover frequency for DDO (2.43 min −1 ) on the Ni/r-TiO 2 catalyst reduced at 650 °C was ∼40 and ∼14 times higher than that of Ni on rutile and anatase, respectively, reduced at 350 °C. This study provides an example of “Goldilocks principle” in catalysis, i.e., the best performing catalyst offers a balanced SMSI!
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Advanced Optical Materials
·
2021
·Vol. 9
·期 24
·2101333
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IF 9.926
Kunjie Liu,Chenkai Deng,Chunxiao Li,Xusheng Zhang,Jindong Cao,Jiyong Yao,Jing Zhao,Xingxing Jiang,Zheshuai Lin,Quanlin Liu
Organic–inorganic metal halides (OIMHs) with unique structural flexibility possess excellent photoelectric properties. They are regarded as next-generation photovoltaic materials, phosphors, semiconductors, and ferroelectrics. The metal-halide units in OIMHs are good microscopic building blocks of nonlinear optical crystals for laser wavelength conversion. However, most OIMHs are absent from nonlinear optics owing to their macroscopic nonlinear optical (NLO)-inactive centrosymmetric crystal structure. In this study, two new lead-free OIMHs, (TMEDA)SbI 5 and (TMEDA)BiI 5 (where TMEDA 2+ is N , N , N ′-trimethylethylenediammonium), having 1D structure, crystallized in the orthorhombic system with a non-centrosymmetric P 2 1 2 1 2 1 space group, are synthesized. Remarkably, upon 2090 nm laser irradiation, both compounds possess a strong infrared (IR) nonlinear optical response of the same magnitude as AgGaS 2 , which is a benchmark semiconductor-type nonlinear optical crystal. In addition, under the excitation of ultraviolet and visible lights, both compounds produce self-trapped exciton-induced red-light emission. First-principles electronic structure calculations reveal that the optical properties originate from the electronic transitions within the inorganic metal-halide group. The obtained results indicate that both compounds are potential photoelectric materials for laser frequency conversion and fluorescence, and the observation of NLO effect in these two compounds verifies that OIMHs are also good candidates for NLO crystals.
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INORGANIC CHEMISTRY
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2021
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IF 5.165
Hang Ruan,Zhongnan Guo,Jiawei Lin,Kunjie Liu,Lingling Guo,Xin Chen,Jing Zhao,Quanlin Liu,Wenxia Yuan
The Pb-free hybrid-layered-double perovskites (HLDPs) have been proposed as green and stable semiconducting materials for optoelectronic devices, but the synthesized members are still limited. Here, we report the synthesis of three new HLDPs, (C8H20N2)2AgMBr8 (M = In, Sb, and Bi), by a solution method using 1,4-bis(ammoniomethyl)cyclohexane (C8H20N22+) as the organic spacing cation. All three of these HLDPs show ⟨100⟩-oriented layered structures with Ag and In/Sb/Bi order arranged in corner-sharing octahedral layers. The first-principle calculations indicate the indirect-gap nature of (C8H20N2)2AgInBr8 and (C8H20N2)2AgSbBr8, while their Bi counterpart shows a direct band gap after considering spin–orbit coupling. The band gaps obtained by diffuse-reflectance spectroscopy are 3.11, 2.60, and 2.70 eV for M = In, Sb, and Bi, respectively. (C8H20N2)2AgInBr8 shows a broadband red emission centered at 690 nm, and it is mainly attributed to the self-trapped-excitons mechanism. Our results not only provide a series of new “Pb-free” HLDPs with chemical diversity but also help us to further understand the structure–property relationships of HLDP materials.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Yi Yang,Huiping Zhang,Haoxin Huang,Ying Yan,Xinya Zhang
Degradation of organic pollutant through catalytic wet peroxide oxidation (CWPO) is becoming more and more important in modern industry. As a commonly used organic synthetic material, excessive discharge of m-cresol may lead to severe damage of the environment and become a potential threat to human health. In this study, m-cresol was degraded over novel iron loaded carbon nanotube microfibrous composite (Fe-CNT-MF) catalyst packed fixed bed reactor. The kinetic parameters were first optimized, and then the deactivation mechanism of catalyst was also studied. The optimization model showed that total organic carbon (TOC) conversion of m-cresol degradation can reach about 70% under optimum conditions. Then the catalyst deactivation test was conducted with four consecutive runs (32 h in total). Fe-CNT-MF performed high m-cresol and TOC conversions (99% and 40%, respectively) as well as high H 2 O 2 decomposition efficiency (100%) with no iron leaching. Besides, the effect of co-existing organic pollutants on m-cresol degradation was investigated with presence of 4-Ethylphenol and 2,5-dimethylphenol. Fe-CNT-MF exhibited good catalytic activity in multi-pollutant wastewater with 99% conversion for all pollutants. Finally, deactivation analysis results showed that the deactivation mechanism of Fe-CNT-MF included carbon deposition, surface property change and additional oxygen functionalities. A regeneration study was proceeded to further confirm the suggested mechanism, indicating that Fe-CNT-MF has a good regenerability.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2020
·Vol. 31
·期 24
·22375-22384
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IF 2.22
Wang Li,He Lin,Li Ji,Yu Yongsheng,Li Haibo
M-type strontium ferrite is a kind of magnetic functional material with wide application prospect. In this work, SrFe 12− x Al x O 19 (0 ≤ x ≤ 1) and Sr 1− y Ca y Fe 8 Al 4 O 19 (0 ≤ y ≤ 0.4) have been prepared by a hydrothermal method, and the effects of Al 3+ doping and Al 3+ and Ca 2+ co-doping on the magnetic properties have been investigated. X-ray diffraction analysis indicates all the samples are a hexagonal structure, and the shift of the diffraction peaks suggests that Al 3+ and Ca 2+ are successfully doped in SrFe 12 O 19 . Field emission scanning electron microscope images show the particles have the hexagonal shape with the size of 1.1–2.9 µm. Vibrating sample magnetometer reveals that the doping of Al 3+ and the co-doping Al 3+ and Ca 2+ can enhance magnetic properties of strontium ferrite. For example, the values of coercivity and the saturation magnetization of SrFe 8 Al 4 O 19 are 914.1 Oe and 44.0 emu/g, which are 3% and 117% enhancement compared with SrFe 12 O 19 , respectively. For Sr 1− y Ca y Fe 8 Al 4 O 19 , coercivity and saturation magnetization increase from 914.1 Oe and 41.8 emu/g to 1047.2 Oe and 50.2 emu/g when the Ca 2+ doping concentration increases from 0 to 0.4. Moreover, the effects of acid washing also on phase composition, morphology and magnetism are researched. The as-synthesized doping strontium ferrite will be useful for the applications in security switching and recording media.
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RSC Advances
·
2020
·Vol. 10
·期 8
·4554-4560
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IF 3.119
Su Xunwen,Zhu Liqun,Li Weiping,Liu Huicong,Ye Hui
CeO2/polymer nanoparticles have drawn considerable attention for their excellent UV absorption properties. However, many challenges still exist in the successful incorporation of ceria into the polymer matrix for the easy agglomeration and photocatalytic activity of CeO2 nanoparticles. Herein, we address these issues by constructing three-layer structured nanoparticles (M-CeO2@SiO2) and incorporating them into a polymer matrix through a mini-emulsion polymerization process. During this process, small-sized nano-ceria became uniformly anchored on the surfaces of monodisperse silica particles first, and then the particles were coated with an MPS/SiO2 shield. The morphology and dispersion of the nanoparticles were investigated using scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The performance of the hybrid films was characterized using UV-vis absorption spectroscopy (UV-vis) and water contact angle (WCA) measurements. Results showed that the M-CeO2@SiO2 nanoparticles exhibited a three-layer structure with a mean diameter of 360 nm, and they possess good compatibility with acrylic monomers. After the addition of M-CeO2@SiO2, hybrid films exhibited enhanced UV absorption capacity as expected, accompanied by an obvious improvement in hydrophobicity (the water contact angle increased from 84.2° to 98.2°). The results showed that the hybrid films containing M-CeO2@SiO2 particles possess better global performance as compared with those containing no particles.
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