CATALYSIS LETTERS
·
2015
·Vol. 145
·期 10
·1913-1921
·
IF 2.307
Wu Jing,Zhi Yunfei,Shan Shaoyun,Su Hongying,Wu Shuisheng,Jia Qingming
Abstract Polypyrrole(PPy) supported Cr(III)(salen)Cl catalyst was prepared for alternating copolymerization of cyclohexene oxide and carbon dioxide. The supported catalyst and the copolymerization products were characterized by FTIR, XRD, XPS, ICP-MS, SEM, TEM, NMR, gel permeation chromatography, thermogravimetric analysis and differential scanning calorimetry. After the study, we concluded that the homogeneous Cr(III)(salen)Cl is successfully supported on the PPy, and its catalytic performance is much better than the homogeneous one. Moreover, the copolymerization product catalyzed by PPy-Cr(III)(salen)Cl exhibits higher molecular weight, narrower molecular weight distribution, superior thermal stability and selectivity. Graphical Abstract
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EUROPEAN POLYMER JOURNAL
·
2015
·
IF 3.005
Erjun Tang,Kaidi Du,Xiaoyan Feng,Miao Yuan,Shaojie Liu,Dishun Zhao
The pH-responsive cellulose-g-poly[2-(diethylamino)-ethyl methacrylate] (cellulose-g-PDEAEMA) copolymers were successfully synthesized by atom transfer radical polymerization (ATRP) in the ionic liquid 1-allyl-3-methylimidazolium chloride ([AMIM]Cl). As the functional monomer 2-(diethylamino)ethyl methacrylate (DEAEMA) hardly dissolved in [AMIM]Cl, we used ethyl alcohol as the cosolvent to increase its solubility and thereby form a homogeneous system. Compared with the synthetic mechanism for the heterogeneous system, generation of the byproduct poly[2-(diethylamino)ethyl methacrylate] (PDEAEMA) in the homogeneous system was reduced and the ATRP reaction was easily controlled. Optimum reaction condition was attained at the CuBr/PMDETA/DEAEMA/ethyl alcohol molar ratio of 1:15:150:300. Kinetic analysis confirmed the reaction was living and controllable. Cellulose-g-PDEAEMA was characterized through FTIR, 1 H NMR, TEM and GPC. The results showed that the PDEAEMA brush was covalently bonded to the cellulose backbone and its molecular weight distribution was narrow. In addition, the resultant copolymer could self-assemble into spherical micelles and showed the pH-sensitivity, implying its potential application as biomedical materials.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ping Ye,Heng Ding,Bo Yang,Weimiao Wang,Xiaodong Li,Zhiqiang Qiao,Rui Li,Guangcheng Yang,Guoqing Lv
The ignition strategy of energetic materials using low-energy near-infrared (NIR) laser has garnered significant attention due to its enhanced safety and reliability. This study explores the use of a relatively photosensitive but mechanical insensitive energetic material, DATNBI, to facilitate the self-assembly of nano-CL-20 crystals into polycrystalline particles though solvothermal induction, yielding a rough structure conducive to NIR laser ignition. The findings demonstrate that by adjusting the content of DATNBI, it is possible to achieve micro-nano controllable spherical CL-20/DATNBI (C/D) particles, with CL-20 as the primary component and DATNBI as the auxiliary component. The incorporation of DATNBI and the rough surface structure enhance the light absorption of C/D particles in the NIR band. Additionally, the unique synergistic effect between CL-20 and DATNBI during thermal decomposition further promotes NIR laser ignition. As expected, the C/D particles achieved self-sustained combustion and exhibited excellent combustion performance under a 1064 nm laser, which is challenging to be achieved with raw CL-20 or raw DATNBI. Furthermore, the relatively insensitive DATNBI and spherical structure reduced the impact sensitivity of the C/D particles. This multifunctional material strategy, integrating energy, safety, environment-friendliness, and laser ignition performance, offers a novel approach for laser ignition of energetic materials.
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RARE METALS
·
2024
·
IF 9.6
Hu Xiao-Jie,Sun Yu-Han,Liu Ling-Yue,Mao Dan-Jun,Zheng Shou-Rong
Monochloroacetic acid (MCAA) is identified as a highly carcinogenic disinfection by-product in chlorinated drinking water. In this study, a series of CeO 2 -supported Pd catalysts (Pd/MCeO 2 ) were synthesized through one-step calcination of Pd-loaded Ce-UiO-66-BDC (Ce-MOF), and the liquid-phase catalytic hydrodechlorination of MCAA was explored using these catalysts. For comparison, Pd/CeO 2 catalysts were additionally synthesized using the conventional impregnation method. The characterization results reveal that the catalysts exhibit strong metal–support interaction, leading to high Pd dispersion and Pd n + content. Additionally, the calcination temperature significantly influences catalytic performance, with the catalyst calcined at 500 °C (Pd/MCeO 2 -500) demonstrating the highest catalytic activity and achieving complete dechlorination of MCAA within 50 min. Furthermore, it is found that the catalytic MCAA hydrodechlorination using the catalysts adheres to the Langmuir–Hinshelwood model. Accordingly, low reaction pH is favorable for the catalytic hydrodechlorination of MCAA, enhancing MCAA adsorption on the catalyst surface due to the electrostatic interaction between MCAA and the catalyst surface. Theoretical results suggest that the presence of Pd n + efficiently facilitates MCAA adsorption and C–Cl cleavage, thus significantly enhancing the liquid-phase catalytic hydrodechlorination. Graphical abstract
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Advanced Energy Materials
·
2022
·Vol. 12
·期 27
·2201243
·
IF 29.698
Qin Zhou,Chunsheng Cai,Qin Xiong,Zilong Zhang,Jianbin Xu,Lusheng Liang,Shibo Wang,Weihai Sun,Zhongyi Yuan,Peng Gao
In perovskite solar cells (PSCs), defective perovskite grain boundaries (GBs) and/or surface due to photo-excitation and the resulted suboptimal carrier dynamics at the perovskite/charge transport layer, have largely limited further performance enhancement and aggravated the PSCs instability. Fundamentally preventing the formation of these trap-states through a simple and efficient approach is thus critical to the enhancement of both device performance and stability. Herein, a novel semiconductive silicon naphthalocyanine derivative (Cl-SiNcTI) to reduce the deep level trap states at the GBs and the surface of perovskite film is successfully employed via a newly proposed photon-relaxation mechanism. The resulting benign p-type surface polarity and suppressed non-radiation recombination lead to improved charge transport in bulk perovskite and at the perovskite/spiro-OMeTAD interface. With a synergistic contribution of the Cl-SiNcTI and 2-(2-Fluorophenyl)ethylamine iodide (oFPEAI), a 24.30% efficiency is achieved in a single cell with excellent operational stability. Moreover, under steady-state light illumination, 93% power output compared to its initial state can still be maintained after 250 h of continuous operation.
研究领域:
光伏技术
·
材料科学
·
半导体物理
·
可再生能源
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RSC Advances
·
2023
·Vol. 13
·期 9
·5993-6001
·
IF 3.9
Zhi Jiang,Hezhuang Liu,Jihua Zou,Yixuan Huang,Zhaoquan Xu,Denys Pustovyi,Svetlana Vitusevich
High-quality CsCu2X3 and Cs3Cu2X5 (X = Cl, Br, I) nanocrystals (NCs) exhibit excellent optoelectronic, physical, and chemical properties for detection of UV radiation due to large carrier mobility and lifetime, and heavy atoms. The nanocrystal materials can be prepared via a low-cost and simple solid-state synthesis. However, poor reproducibility and complex synthesis methods of obtaining perovskite NC thin films represent a drawback for the fabrication of the commercial photoelectric device. To address these issues, we develop highly stable CsCu2X3 and Cs3Cu2X5 NC materials using a facile solid-state reaction method for the scale-up production of halogen lead-free perovskites. We suggest a distinctive way to design a series of nanocrystalline perovskites using short-term synthesis and study the mechanism of perovskite formation using thermal solid-state synthesis. These all-inorganic and lead-free CsCu2X3 and Cs3Cu2X5 exhibit large photoluminescence quantum yields (PLQYs) up to 95.2%. Moreover, flexible paper photodetectors based on this series of lead-free perovskites show strong photoselectivity and bending stability at 254 nm, 365 nm, and 405 nm wavelengths. High-quality responses with a responsivity of 1.1 × 10−3 A W−1 and detectivity of 2.71 × 109 jones under UV illumination (10 μW cm−2) at a bias voltage of 5 mV are demonstrated. These results open prospects for designing photodetectors, LEDs, and other photosensitive devices.
研究领域:
材料科学
·
光电技术
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高影响因子
Journal of Environmental Chemical Engineering
·
2026
·
IF 7.2
Ning Gao,Yike Yao,Yunbo Wang,Mengjie Fan,Xiaoqian Peng,Yingwen Chen
In high-viscosity, metal salt-based deep eutectic solvents (DESs), strong hydrogen-bonding interactions frequently hinder mass transfer, limit ROS formation, and reduce synergistic catalytic activity. To address these challenges, a low-viscosity DES incorporating Brønsted-Lewis acidic sites was synthesized from FeCl₃·6H₂O and propionic acid. In this configuration, solid PMS acts as a slow-release oxidant, thereby preserving the DES’s functional integrity and sustaining its catalytic efficiency. Characterization and oxidative desulfurization evaluation revealed alternating Fe ion redox states within the DES, along with a dual cyclic reaction pathway involving the regeneration of Cl⁻ and Cl radicals. The electron-transfer activity of Cl radicals not only generates multiple reactive oxygen species (·ClO and ·O 2 ⁻) but also modulates the nucleophilic and electrophilic reactivity of organosulfur compounds. Under mild conditions at 40 °C, the catalytic system achieves over 99.7% desulfurization of model oil containing up to 1500 mg kg -1 sulfur within 20 minutes, while demonstrating excellent recyclability over seven consecutive cycles. DFT analyses indicate that radical oxidation serves as the dominant pathway for thiophene sulfone formation, with perpropionic acid playing an auxiliary role by extending the lifetime of reactive oxygen species and enhancing the oxidation process. Overall, the controlled release of solid PMS reduces impurity effects on the DES, while radicals and reactive oxygen species promote S-O bond formation and the removal of organosulfur compounds from the oil phase.
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Science China-Materials
·
2020
·Vol. 64
·期 1
·158-168
·
IF 6.098
Fang Cong,Li Ye,Cai Yuting,Zhou Tian-Liang,Tang Xueyuan,Xie Rong-Jun
Cesium lead halide perovskite nanocrystals (NCs) have attracted unprecedented attention owing to their compelling properties for optoelectronic applications. Compared with the classical hot-injection method, the room-temperature (RT) synthetic strategy is more facile and tender, but it is hard to obtain stable CsPbI 3 NCs and it usually uses polar solvents that sometimes reduce the stability and properties of NCs. Here, we reported a simple approach to synthesize highly efficient and stable CsPbI 3 as well as other color-tunable CsPbX 3 NCs with high quantum efficiency at room temperature via an anion exchange at the water-oil interface, in which the as-synthesized pristine CsPbBr 3 NCs in toluene were treated in aqueous solutions of HX (X=Cl, Br, and I) and protonated oleylamine (OAm) acted as a carrier. The synthesized CsPbI 3 NCs had an emission at 680 nm and even showed excellent colloidal stability after being stored for 32 d. The high efficiency and stability of the obtained CsPbX 3 NCs were ascribed to the facts that: (i) the polar reagents were almost removed from the surface of NCs; (ii) the defect-related nonradiative recombination was suppressed efficiently by surface passivation.
研究领域:
纳米材料
·
光电子学
·
钙钛矿化学
·
胶体合成
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 23
·7893-7905
·
IF 4
Lingjun Shu,Jingxuan Yin,Zhemin Gon,Chengwei Gao,Yongxing Liu,Xiaolong Zhou,Hongli Ma,Xianghua Zhang,Xiang Shen,Shixun Dai,Changgui Lin,Qing Jiao
The fabrication of all electrolytes from noncombustible ceramic materials offers a superior option for providing safer and higher-capacity batteries to fulfill future energy needs. To achieve a competitive performance with combustible liquid electrolytes used in commercial Li-ion batteries, the creation of ceramic material compositions with a high electrical conductivity is necessary. Here, we report that co-doping with W and halogens results in a superconductivity of 13.78 mS cm−1 in a cubic-phase Na3SbS4 glass ceramic electrolyte. After undergoing high-temperature heat treatments, the W ions in the electrolyte can facilitate the replacement of S atoms with halogens, introducing many Na vacancies. The samples also had a high degree of cycling stability. An excellent glass ceramic electrolyte for Na ion batteries will be constructed for Na3SbW0.25Cl0.25S4.
研究领域:
材料科学
·
电化学
·
固态离子学
·
能源存储
·
无机非金属材料
·
电池技术
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高影响因子
CHEMISTRY OF MATERIALS
·
2022
·
IF 10.508
Ruiwen Ji,Meng Lei,Cécile Genevois,Wenda Zhang,Xing Ming,Lunhua He,Mathieu Allix,Congling Yin,Xiaojun Kuang,Xianran Xing
Layered materials coupling a two-dimensional strong-bonding layered network with much weaker van der Waals (vdW) interaction between the layers are sought after for the development of nanoelectronics and energy conversion devices. It is important to elucidate the layer stacking rules in these vdW materials and control the thickness of the strong-bonding layers for tuning the nanosheet height during exfoliation and therefore tailor physical properties. Here, we show that the single Bi2O2Se ionic layer in the three-anion vdW semiconductor Bi4O4SeCl2 showing extremely low thermal conductivity can be expanded to higher-order layers forming a homologous series Bi2+2nO2+2nSenX2 (X = Cl, Br) with variable ionic layer thicknesses. Bi4O4SeX2 (n = 1) and Bi6O6Se2X2 (n = 2) were isolated as single-phase materials, while materials with larger layer thicknesses such as Bi8O8Se3Cl2 (n = 3) contain different defect-intergrowth structures at the crystallite scale. The anionic disorder of Se and X within the Bi2O2Se and Bi2O2X2 slabs is a critical factor in the stabilization of Bi2+2nO2+2nSenX2. The ∼50% Se substitution by X anions in the Bi2O2Se slab as related to the weak interlayer interaction can serve as a stabilization criterion of Bi2+2nO2+2nSenX2. All of these materials show similar optical indirect band gaps of ∼1.05 eV, originating from the electronic states in the Bi2O2Se slabs. Pellets prepared from these vdW materials possessed low bulk resistivities (100 Ω·cm) and exceptionally low and tunable thermal conductivities (0.66 W/mK and lower) parallel to the pressing axis of the pellets (heavier the halogen is, lower is the thermal conductivity). The results presented here provide important multiple anion chemistry for tailoring the ionic-bonding network into different thicknesses in the vdW layered structures and therefore their physical properties.
研究领域:
材料科学
·
化学
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高影响因子
ACS Applied Nano Materials
·
2026
·
IF 5.8
Yan Yuxin,Zou Ailing,Wang Yiyan,Zhang Yanjie,Yu Jingjie,Xiao Zhiguo
CsPbX 3 (X = I, Br, Cl) perovskite quantum
dots (PQDs)
are promising for optoelectronic applications owing to their tunable
bandgap, high photoluminescence (PL) quantum yield, and narrow emission
bandwidth. However, CsPbBr 3 PQDs exhibit a large Stokes
shift (>155 nm) and are mainly excited by near-ultraviolet light
(∼365
nm), resulting in substantial energy loss and limiting their compatibility
with blue light-emitting diodes (LEDs) excitation. Herein, Sr 2+ /Cl – codoped CsPbBr 3 PQDs embedded
in zinc borosilicate (ZBS) glass powders were developed to regulate
the band structure. Sr 2+ incorporation significantly enhances
PL performance. Notably, CsPb 0.5 Sr 0.5 Br 3 PQDs exhibit ∼1.6 times higher PL intensity than undoped
samples with a slight red-shift (∼5 nm). Meanwhile, the bandgap
of CsPb 0.1 Sr 0.9 Br 3 PQDs is widened
to 3.12 eV compared to 2.36 eV for CsPbBr 3 . Totally different
with undoped PQDs, the excitation peak of CsPb 0.1 Sr 0.9 Br 3 PQDs covers the desired blue-violet region
in the range of 400–480 nm and the maximum peak is located
at 414 nm, which displays a narrow Stokes shift of 106 nm. Further,
Cl – ions substitution in Sr-doped host materials
enables the blueshift of the PL emission from 521 nm (green light)
to 448 nm (blue light) via bandgap engineering accompanied by ultranarrow
Stokes shift of ∼34 nm for CsPb 0.1 Sr 0.9 BrCl 2 sample. The Sr-doped PQDs embedded in ZBS glass
also demonstrate excellent water resistance, retaining ∼96%
of their initial PL intensity after immersion in deionized water for
more than 60 days. Thus, the ultrastable PQDs glass powders can be
effectively excited by the blue-violet light chip (410 nm-460 nm)
via bandgap engineering possess and demonstrate promising application
potential in color-conversion display devices, wide-color-gamut backlight
systems and screen-printable emissive display films.
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Science China-Chemistry
·
2025
·
IF 9.7
Kang Kai,Wang Qiuxiang,Huang Hongpu,Zhuang Xinxin,Cai Junlin,Wang Tao,Wang Xue,Xie Zhaoxiong,Xie Shuifen
Despite utilization of state-of-the-art Cu-based catalysts, achieving high selectivity and stability in multicarbon (C 2+ ) compounds production through electrocatalytic CO 2 reduction reaction (CO 2 RR) remains a critical and challenging objective. Here we employ lattice chlorine-doped Cu 2 O nanocubes (Cl d -Cu 2 O NCs) with well-defined {100} facets as a model catalyst to demonstrate that halogen doping can serve as a versatile and effective strategy for modulating surface charge distribution, thereby enhancing asymmetric C–C coupling toward high-selectivity C 2+ products in CO 2 RR. Compared to Cl-free Cu 2 O NCs, Cl d -Cu 2 O NCs exhibit a greatly enhanced C 2+ Faraday efficiency, i.e., ∼85% at −1.1 V (versus the reversible hydrogen electrode). Additionally, the Cl d -Cu 2 O NCs demonstrate significantly enhanced long-term durability, attributed to better preservation of the cubic morphology and more stable Cu δ + states. In-situ electrochemical studies reveal that Cl d -Cu 2 O NCs facilitate the formation of the key asymmetric *COH and *OCCOH intermediates, ultimately leading to higher C 2+ products. Density functional theory (DFT) calculations confirm that the introduced Cl-dopants disrupt the charge balance of the Cu 2 O(100) surface, enriching the Cl-adjacent Cu atoms with more electrons compared to those near O atoms. This unbalanced charge distribution significantly reduces the free energy of the rate-determining step for asymmetric C–C coupling from the *CO to *OCCOH on Cl-doped Cu 2 O (100) surface, requiring only 1.04 eV, in contrast to 1.50 eV on pristine Cu 2 O(100) surface. This study provides valuable insights into the surface charge modulation of Cu 2 O catalysts via halogen doping for enhancing asymmetric C–C coupling and C 2+ production in CO 2 RR.
研究领域:
电催化
·
材料科学
·
环境化学
·
纳米技术
·
物理化学
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