JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2024
·Vol. 35
·期 26
·1-11
·
IF 2.8
Li Xiao-Bing,Ma Xiao-Ye,Zhang Xue-Feng,Jia Guo-Liang,Zhao Zhao-Ye,Wang Jun-Chuan,Wang Hui,Wu Xiang-Feng
In this work, PCN-224(Fe) porphyrin-based metal–organic frameworks and a Poly(ionic liquids) (PILs) were used to prepare PCN-224(Fe)@PIL(Cl − ) composite films by UV polymerisation. The structure, morphology, chemical composition, and electrochemical properties of the as-prepared composite film were investigated. PCN-224(Fe) was coated with a kind of P(1-vinylpyridinium chloride as monomer) on the outside to improve the electron transfer efficiency, while an electrochemical system was employed to catalysis the persulfate (PS) decomposition for the efficient degradation of tetracycline (TC). Because of the cathodic reduction reaction, the continuous redox cycle between Fe 3+ /Fe 2+ was facilitated, which enhanced the degradation activity of persulfate on tetracycline. The PCN-224(Fe)@PIL(Cl − ) composite demonstrated a superior electrocatalytic degradation efficiency of 95.8% in just 40 min for the TC model pollutant, surpassing the 63.3% efficiency of pure PCN-224(Fe) within 60 min. This work shows a successful example of using PILs to enhance catalytic degradation activity and points out a direction of preparation of catalysts for activating persulfate (PS).
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ACS Earth and Space Chemistry
·
2024
·
IF 2.9
Cici Fan,Weigang Wang,Bo Shi,Zheng Sun,Maofa Ge
The relative rate method was used to determine the rate constant of Cl atoms and 3-buten-1-ol at ambient temperature and pressure. The main products of the reaction were identified as HCOOH with a yield of (50.07 ± 2.65)%, HCHO with a yield of (18.24 ± 0.65)%, HOCH2CHO with a yield of (18.69 ± 0.68)%, ClCH2CHO with a yield of (7.64 ± 0.25)%, respectively. The rate constant was (3.04 ± 0.36) × 10–10 cm3 molecules–1 s–1. The calculated theoretical rate constant was 2.91 × 10–10 cm3 molecules–1 s–1, which was in agreement with the experimental results. Moreover, the theoretical calculation showed that the two Cl-addition pathways were the main reaction pathway, but the proportion of H-abstraction pathways reached 29%, and its importance cannot be ignored. Based on this, the possible reaction mechanisms were deduced. The atmospheric implications of the obtained title reaction were briefly discussed.
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ACS Omega
·
2024
·
IF 3.7
Ruonan Yao,Jiawei Lin,Kunjie Liu,Yuanchang Xu,Boyi Xiao,Jing Zhao,Zhongnan Guo,Quanlin Liu,Wenxia Yuan
Low-dimensional tin-based halide perovskites are considered as eco-friendly substitutions of the iconic lead-based perovskites to host the potential as optoelectronic materials. However, a fundamental understanding of the structure–property relationship of these Sn(II)-based hybrids is still inadequate due to the limited members of this material family. To our knowledge, there is still lack of reports on a series of Sn(II)-based halide perovskites with the same organic cation but covering chloride, bromide, and iodide. In this work, three new halide perovskites TMPDASnX4 (X = Cl, Br, I) (TMPDA = N,N,N′,N′-tetramethyl-1,4-phenylenediamine) are successfully synthesized, which provide the ideal paradigm to study the halogen-dependent evolution of the structure and properties of Sn(II)-based hybrid perovskites. Despite sharing the same monoclinic lattice (P21/m space group), it is demonstrated that TMPDASnCl4 adopts a one-dimensional structure composed of a five-coordinated pyramid configuration due to an extremely long Sn···Cl distance, while the typical two-dimensional motif is still maintained in TMPDASnBr4 and TMPDASnI4. The ambient stability is declined in the order from chloride to bromide and then to iodide. TMPDASnCl4 exhibits a broad-band bluish-white-light emission (centered at 515 nm, full width at half-maximum (fwhm) = 193 nm) with the Commission Internationale de l′ Elairage (CIE) coordinates as (0.29, 0.34). Further, the correlated color temperature and color-rendering index were determined as 7617 K and 80.5, respectively. Based on the synthesis of new crystals, our work sheds light on the composition–structure–property relationship of hybrid Sn(II)-based halide perovskites.
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ADVANCED MATERIALS
·
2015
·Vol. 27
·期 35
·5176-5183
·
IF 17.493
Liu Y,Yang Z,Cui D,Ren X,Sun J,Liu X,Zhang J,Wei Q,Fan H,Yu F,Zhang X,Zhao C,Liu SF.
Two-inch-sized perovskite crystals, CH3 NH3 PbX3 (X=I, Br, Cl), with high crystalline quality are prepared by a solution-grown strategy. The availability of large perovskite crystals is expected to transform its broad applications in photovoltaics, optoelectronics, lasers, photodetectors, LEDs, etc., just as crystalline silicon has done in revolutionizing the modern electronics and photovoltaic industries.
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FOOD CHEMISTRY
·
2019
·
IF 5.399
Xiupei Yang,Jing Xu,Na Luo,Fenglin Tang,Maoxue Zhang,Bin Zhao
Chemical doping with heteroatoms was employed to prepare N,Cl co-doped fluorescent carbon dots (N,Cl-FCDs) which may be designed for the detection of tartrazine. Using urea as the N source and FeCl 3 · 6H 2 O as the Cl source, N,Cl-FCDs were synthesized by hydrothermal method with carbon dots prepared from aloe. Compared with pure carbon dots (CDs), N,Cl-FCDs resulted in dramatic improvement in the fluorescence properties and surface physical chemical properties. The fluorescence quantum yield of the N,Cl-FCDs was as high as 60.52%. As an effective fluorescence probe for tartrazine, a good linear relationship between N,Cl-FCDs and tartrazine was constructed at the concentration range from 0.1 to 30 μM with a detection limit of 48 nM based on the mechanism of fluorescence resonance energy transfer (FRET). The proposed fluorescent probe method was successfully applied to detect tartrazine in beverages, which is expected to have a potential application in the field of food analysis.
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Journal of the American Chemical Society
·
2020
·
IF 14.612
Xianju Zhang,Xianxin Wu,Xiaoyu Liu,Gaoyu Chen,Yongkai Wang,Jianchun Bao,Xiangxing Xu,Xinfeng Liu,Qi Zhang,Kehan Yu,Wei Wei,Jingjing Liu,Jun Xu,Hua Jiang,Peng Wang,Xun Wang
Perovskite and chalcogenide quantum dots (QDs) are important nano semiconductors. It has been a challenge to synthesize heterostructural QDs combining perovskite and chalcogenide with tailorable photoelectronic properties. In this report, heterostructural CsPbX3-PbS (X = Cl, Br, I) QDs were successfully synthesized via a room temperature in situ transformation route. The CsPbX3-PbS QDs show a tunable dual emission feature with the visible and near-infrared (NIR) photoluminescence (PL) corresponding to CsPbX3 and PbS, respectively. Typically, the formation and evolution of the heterostructural CsPbBr3–PbS QDs with reaction time was investigated. Femtosecond transient absorption spectroscopy (TAS) was applied to illuminate the exciton dynamics in CsPbBr3–PbS QDs. The mild synthetic method and TAS proved perovskite to PbS energy transfer may pave the way toward highly efficient QD photovoltaic and optoelectronic devices.
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NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 39
·16877-16890
·
IF 3.288
Xiangbo Song,Chenguang Wang,Lungang Chen,Qiying Liu,Jianguo Liu,Yuting Zhu,Jun Yue,Longlong Ma
Ionic liquids (ILs) as additives were used in the selective conversion of bio-based carbohydrates to 5-hydroxymethylfurfural (HMF) in this work. The effect of adding various imidazole-based ionic liquids with different anion structures on the production of HMF from fructose was firstly investigated in aqueous media. The presence of 15 wt% 1-butyl-3-methylimidazole chloride ([Bmim]Cl) ionic liquids in water with Fe2(SO4)3 as the homogeneous catalyst provided a more effective HMF synthesis compared to that without [Bmim]Cl addition. The enhanced HMF yield was mainly attributed to the fact that [Bmim]Cl might play a vital role in stabilizing the HMF molecule, which could thereby suppress side reactions involving HMF (e.g., its rehydration to levulinic acid or/and polymerization to humins). NMR and FTIR analyses suggested that such a stabilization effect stemmed from the interaction of [Bmim]Cl with the hydroxyl and aldehyde groups of HMF through hydrogen bonding. By performing the operation in a biphasic system (i.e., with the biomass-derived THF solvent as the organic phase and the addition of NaCl salt into water for improving HMF partition), the HMF yield over the Fe2(SO4)3 catalyst in the presence of the [Bmim]Cl additive could be further improved. The catalyst and ionic liquids were quite stable, and could be reused for more than five cycles with a consistent activity. A similar enhancement effect of [Bmim]Cl was also demonstrated in HMF synthesis with better yields from other biomass feedstocks or derivatives (including glucose, sucrose, cellobiose, inulin and starch) in aqueous media.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Su Han,Li Jingru,Zhong Yu,Liu Yu,Gao Xuhong,Kuang Juner,Wang Minkang,Lin Chunxi,Wang Xiuli,Tu Jiangping
Sulfides are promising electrolyte materials for all-solid-state Li metal batteries due to their high ionic conductivity and machinability. However, compatibility issues at the negative electrode/sulfide electrolyte interface hinder their practical implementation. Despite previous studies have proposed considerable strategies to improve the negative electrode/sulfide electrolyte interfacial stability, industrial-scale engineering solutions remain elusive. Here, we introduce a scalable Li-Al-Cl stratified structure, formed through the strain-activated separating behavior of thermodynamically unfavorable Li/Li 9 Al 4 and Li/LiCl interfaces, to stabilize the negative electrode/sulfide electrolyte interface. In the Li-Al-Cl stratified structure, Li 9 Al 4 and LiCl are enriched at the surface to serve as a robust solid electrolyte interphase and are diluted in bulk by Li metal to construct a skeleton. Enabled by its unique structural characteristic, the Li-Al-Cl stratified structure significantly enhances the stability of negative electrode/sulfide electrolyte interface. This work reports a strain-activated phase separation phenomenon and proposes a practical pathway for negative electrode/sulfide electrolyte interface engineering.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2019
·
IF 7.149
Yu Lei,Shuangshuang Cheng,Na Luo,Xin Yang,Taicheng An
Cl• and Cl2•– radicals contribute to the degradation of trace organic contaminants (TrOCs) such as pharmaceutical and personal care products and endocrine-disrupting chemicals. However, little is known about their reaction rate constants and mechanisms. In this study, the reaction rate constants of Cl• and Cl2•– with 88 target compounds were determined using laser flash photolysis. Decay kinetics, product buildup kinetics, and competition kinetics were applied to track the changes in their transient spectra. Cl• exhibited quite high reactivity toward TrOCs with reaction rate constants ranging from 3.10 × 109 to 4.08 × 1010 M–1 s–1. Cl2•– was less reactive but more selective, with reaction rate constants varying from <1 × 106 to 2.78 × 109 M–1 s–1. Three QSAR models were developed, which were capable of predicting the reaction rate constants of Cl2•– with TrOCs bearing phenol, alkoxy benzene, and aniline groups. The detection of Cl•-adducts of many TrOCs suggested that Cl• addition was an important reaction mechanism. Single electron transfer (SET) predominated in reactions of Cl• with TrOCs bearing electron-rich moieties (e.g., sulfonamides), and their cation radicals were observed. Cl• might also abstract hydrogen atoms from phenolic compounds to generate phenoxyl radicals. Moreover, Cl• could react with TrOCs through multiple pathways since more than one transient intermediate was detected simultaneously. SET was the major reaction mechanism of Cl2•– reactions with TrOCs bearing phenols, alkoxy benzenes, and anilines groups. Cl2•– was found to play an important role in TrOC degradation, though it has been often neglected in previous studies. The results improve the understanding of halogen radical-involved chemistry in TrOC degradation.
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INORGANIC CHEMISTRY
·
2021
·
IF 5.165
Mao-Yin Ran,Sheng-Hua Zhou,Wenbo Wei,Bang-Jun Song,Yong-Fang Shi,Xin-Tao Wu,Hua Lin,Qi-Long Zhu
Inorganic chalcohalides are attracting a tremendous amount of attention because of their remarkable structural variety and desirable physical properties. Although great advances have been made in recent years, functional inorganic chalcohalides with two-dimensional neutral layers are still rare. Herein, two novel chalcohalides CdSnSX2 (X = Cl or Br) with high yields were obtained by reacting CdX2 with SnS using a traditional solid-state method at 823 K. Both of these chalcohalides adopt orthorhombic space group Cmcm (No. 63) with the following structural values: a = 4.014(4)–4.064(2) Å, b = 12.996(2)–13.746(3) Å, c = 9.471(2)–9.621(2) Å, V = 494.1(8)–537.5(2) Å3, and Z = 4. The prominent architectural feature is the unique two-dimensional [CdSnSX2] neutral layer consisting of composite [CdX2] and [SnS] sublattices that are connected alternately through the Cd–S–Sn bonds along the ac plane. The [CdX2] sublattice consists of a single octahedral chain of Cd-centered [CdX4S2] groups sharing cis-X edges, while the [SnS] sublattice consists of a bend-shaped chain of unusual [SnS2X2] units sharing vertices of S atoms. Significantly, each CdSnSX2 form (X = Cl or Br) shows high visible-light-induced photocatalytic activity for rhodamine B degradation, which is ∼7.0 times higher than that of nitrogen-doped TiO2 (TiO2–xNx) under the same experimental conditions. This discovery enriches the categories of inorganic chalcohalides and provides more choices of candidate materials for photocatalytic applications.
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JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY
·
2021
·Vol. 21
·期 12
·6073-6081
·
IF 0
Zhang Qian,Wang Bingxin,Hong Jun-Ming
The application of electrochemical catalytic oxidation in wastewater treatment with powerful Cldoped graphene as an anode has been discussed as a novel approach to degrade acetaminophen effectively. The characteristics of Cl-doped graphene that were related to Cl loading content and
microscopic morphology were analyzed by using several instruments, and the defects created by Cl doping were identified. Quenching experiments and electron paramagnetic resonance detection were proposed to clarify the mechanism underlying the production of active free radicals by Cldopedgraphene.
The degradation results indicated that efficiency increased with the percentage of Cl atoms doped into the graphene. The best degradation efficiency of acetaminophen could reach 98% when Cl-GN-12 was used. In the process of electrocatalytic oxidation, O•−
2,
and active chlorine, as the main active species, persistently attacked acetaminophen into open-ring intermediates, such as 4-chlororesorcinol, and finally into CO2 and H2O.
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Nature Communications
·
2026
·
IF 18.1
Yu Yang,Zhou Wei,Yuan Junshu,Zhou Xiaohan,Zhang Xuewei,Li Xuhan,Xia Xiao,Zhang Liqiang,Chen Yingjian,Meng Xiaoxiao,Wang Xingxing,Sun Fei,Gao Jihui,Zhao Guangbo
From the perspective of sustainable energy and green hydrogen, the critical challenge in seawater electrolysis lies in suppressing competitive chloride oxidation and corrosion at the anode. Despite the proposed protection mechanism based on surface reconstruction-derived anion repellence, a fundamental question of selectivity remains: why does the protective layer exclude Cl - but not the formally equivalent OH - ? We now redefine the connection between reconstruction and interfacial protection in NiFeS anodes to elucidate the origin of underlying selectivity. In-situ Raman, in-situ X-ray absorption spectroscopy, and molecular dynamic calculations further confirm that the reconstructed SO 4 2- establishes an enhanced hydrogen-bond network. This network significantly weakens the hydrogen-bonding strength of Cl - relative to H 2 O, thereby enhancing the discrimination between OH - and Cl - . In practical application, NiFeS demonstrates energy-saving seawater splitting performance (261.8 mV @ 100 mA·cm -2 ), long-term durability (2000 h @ 1.0 A·cm -2 ), and enables stable intermittent electrolysis (1500 start-stop cycles @500 mA·cm -2 ). When integrated into an anion exchange membrane cell, it shows promising electrolysis performance for industrial applications (1.970 V @ 1.0 A·cm -2 ).
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