Catalysis Science & Technology
·
2022
·Vol. 12
·期 6
·1968-1977
·
IF 6.177
Yiwen Yang,Haifeng Qi,Zhanwei Xu,Z. Conrad Zhang
In this work, we identified the prevailing catalytically active species evolved from paired PdCl2–CuCl2 in 1-butyl-3-methylimidazolium chloride ([BMim]Cl) that displayed dramatic synergy between the two metal chlorides in catalyzing the hydrolysis of β-1,4-glycosidic bonds in cellulose. Ultraviolet-visible (UV-vis), far infrared (FIR), and electron paramagnetic resonance (EPR) spectroscopy provide clear evidence for the prominent evolutionary pathways to form the catalytically active species. It is observed that the strong synergy between [PdIICl4]2− and [CuIICl4]2− is initiated by the presence of a saccharide. In the absence of a saccharide, the spectroscopic features of [PdIICl4]2− and [CuIICl4]2− in their paired solution show little change with respect to those of individual metal chloride solutions. The evolution of a highly active heterometallic PdII–Cl–CuI complex from paired PdCl2–CuCl2 in the presence of saccharides is revealed by the transition of the FIR absorption peak of PdII–Cl. Glycolaldehyde as the simplest model compound, which is the same as the reducing end group of saccharides, is applied to determine the possible catalytic species. X-ray absorption spectroscopy (XAS) verifies that [CuIICl4]2− is reduced to [CuICl3]2− by glycolaldehyde. The HCl generated from reduced [CuIICl4]2− is also found to contribute to the hydrolysis of cellobiose, serving as another catalytically active species in paired PdCl2–CuCl2/[BMim]Cl. Paired PdCl2–CuCl2 pretreated with glycolaldehyde exhibits dramatically higher activity than direct use of paired PdCl2–CuCl2 in cellobiose conversion. Strikingly, the PdII–Cl–CuI complex is found to be substantially more active than HCl in the hydrolysis of β-1,4-glycosidic bonds as evidenced by the sustained high cellobiose conversion after neutralization of HCl with NaOH.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Dayong He,Chao Wang,Rui Zhao,Xiaofeng Lu,Mei Yang,Ju Qiu,Kaizhong Wang,Ce Wang
Facing high-energy radiation exposure in many different situations, researchers are focused on developing personal protective equipment against high-energy rays. The design and fabrication of low-density, self-standing, nontoxic, and flexible high-energy ray shielding materials have always been a hot issue in the special equipment manufacturing industry. As key raw materials for high-efficiency X-ray shielding, high-Z element compounds are nonrenewable resources. Therefore, their development and application require far-sighted arrangement. In this work, we demonstrate an easy and general fabrication route of multifunctional high-Z element compounds/polymer nanofibrous membranes through electrospinning and subsequent solvothermal and successive ionic layer adsorption and reaction processes. The as-fabricated BiOX (X = Cl, Br, I)/WO3/PAN nanofibrous membrane exhibits an excellent X-ray shielding capability with a mass attenuation coefficient of 3.55 cm2 g–1 at 83 keV and could achieve a balanced shielding performance by the introduction of inexpensive iodine elements. Additionally, the self-standing hybrid nanofibrous membrane also exhibits remarkable visible-light photocatalytic activities to degrade RhB in aqueous solution, showing potential in water treatment application and providing an efficient and economical route for the development, usage, recycling, and reuse of precious high-Z material-based composites.
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Inorganic Chemistry Frontiers
·
2022
·Vol. 9
·期 18
·4705-4713
·
IF 7.779
Ting Zheng,Qiang Wang,JinXuan Ren,Liling Cao,Ling Huang,Daojiang Gao,Jian Bi,Guohong Zou
Generally, phosphates are employed to design ultraviolet nonlinear optical crystals. However, phosphates always suffer from too small birefringence to effectively achieve phase matching. Herein, the Sn2+ cation with a stereochemically active lone pair was introduced into a phosphate as a birefringence-active unit, and two tin phosphate halides Sn2PO4X (X = F, Cl) were successfully synthesized. Interestingly, the different coordination environments of the Sn-polyhedron caused by the partial substitution of halide ions (F−/Cl−) with different ionic radii for the oxygen ligands lead to structural transformation from centrosymmetric (CS) Sn2PO4F to noncentrosymmetric (NCS) Sn2PO4Cl. Thus, Sn2PO4X (X = F, Cl) were characterized by enlarged birefringence, and Sn2PO4Cl is type I phase-matchable with a moderate SHG response, and is a potential ultraviolet nonlinear optical material. Furthermore, both phosphates show wide band gaps. Theoretical analysis confirmed that their excellent optical properties result from the synergistic effect of the [SnOX] (X = F, Cl) polyhedra with stereochemically active lone pairs and the [PO4]3− tetrahedron.
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Nanomaterials
·
2022
·Vol. 12
·期 12
·2026
·
IF 5.719
Weizhuo Zhang,Xin Li,Chencheng Peng,Fei Yang,Linyuan Lian,Runda Guo,Jianbing Zhang,Lei Wang
Colloidal cesium lead halide (CsPbX3, X = Cl, Br, and I) perovskite nanocrystals (NCs) demonstrate supreme optical properties in the spectra region of infrared, red, and green. High-performance blue-emitting counterparts are still eagerly required for next-generation full-color displays. However, it is challenging to obtain efficient blue perovskite NCs, especially in a deep blue region with an emission wavelength of around 460 nm or shorter. Herein, calcium halide and ammonium ions are applied simultaneously to modify the CsPb(Br/Cl)3NCs in situ to reduce surface defects, finally remarkably enhancing the photoluminescence quantum yield (PLQY) from 13% to 93% with an emission peak at 455 nm and the Commission Internationale de l’Eclairage (CIE) coordinates at (0.147, 0.030), which is close to the requirement of the Rec.2020 standard and also meets the requirement of blue emission in DCI-P3. Bright white emission and a wide color gamut are also achieved by combining the commercial red-emitting and green-emitting phosphors. The combination of time-resolved PL spectra and femtosecond transient absorption results discloses the reason for PLQY improvement as suppressing the nonradiative recombination.Keywords:CsPb(Br/Cl)3nanocrystals;surface passivation;blue emission;ammonium ion;calcium
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INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Qiang Huang,Changqing Tian,Junan Lai,Fei Qi,Nan Zhang,Jiaxin Liu,Zhiyu Liang,Daofu Wu,Xiaosheng Tang
In response to calling for a sustainable and carbon-neutral economy, the conversion of CO2 to useful chemicals using the solar energy is a potential tactic to relieve the global energy dilemma and environmental issues, which has been a hot topic so far. Recently, the lead halide perovskites as novel photocatalysts have attracted researchers’ interests. However, they generally encounter poor stability and lead toxicity, restricting their large-scale practical applications. Here, the lead-free Cs2TeX6 (X = Cl, Cl0.5Br0.5, Br, Br0.5I0.5, and I) perovskite microcrystals with strong stability were prepared and used to realize the CO2 photocatalytic reduction efficiently. The prepared Cs2TeBr6 microcrystals delivered stronger photocatalytic ability than many previously reported photocatalysts, with the CO and CH4 yields of 308.63 and 60.42 μmolg–1, respectively, under 3 h of illumination. The presented strategy in our work provides new ideas of designing and preparing efficient and practical CO2 reduction photocatalysts based on nonleaded and high-stability halide perovskites.
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Journal of Materials Chemistry C
·
2021
·Vol. 9
·期 15
·5182-5189
·
IF 7.393
Liang Bao,Wenqiang Liu,Yonghua Chen,Yanbo Zhang,Yang Zhang
The local surface plasmon resonance effect induced by metal nanoparticles on perovskites provides a powerful approach to enhance the photoluminescence of such all-inorganic systems. Here, we show that the decoration of CsPb(Br/Cl)3 nanocrystals (NCs) with Au nanoparticles (NPs) leads to a significant enhancement of the blue emission centered at 465 nm, resulting in a photoluminescence quantum yield (PLQY) of up to 73%. Our simulations based on finite difference time domain (FDTD) analysis indicate that the distance between the Au NPs and CsPb(Br/Cl)3 NCs plays a crucial role in determining the local electric field intensity. Our data suggest that an excessive decoration of CsPb(Br/Cl)3 NCs with Au NPs can also reduce the PLQY, as a result of decreased coupling strength.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Jiafu Li,Jiahui He,Md. Tareq Aziz,Xiaocui Song,Ying Zhang,Zhiguang Niu
As a well known endocrine-disrupting and model chemical, bisphenol A (BPA) may pose a serious threat to human health, since it and its disinfection by-products (DBPs) have been detected in drinking water , urine, human colostrum, adipose tissue , and placenta samples. Although chlorinated BPAs (Cl-BPAs) and iodinated BPAs (I-BPAs) have been well studied, brominated BPAs (Br-BPAs), and mixed halogenated DBPs like bromo-iodo-BPAs (Br-I-BPAs), and bromo-chloro-iodo-BPAs (Cl-Br-I-BPAs) are less well understood. Notably, the role of iodide (I - ) during chlorination is not well understood, since the studies of the I-DBPs mainly focus on their genotoxicity and cytotoxicity. To understand the formation mechanisms of halogenated bisphenol A (HBPs) during chlorination with bromide (Br - ) and/or I - , and the role of I - during chlorination, three set of reactions were performed in the laboratory (“BPA + chlorine + Br - ”, “BPA + chlorine + I - ” and “BPA + chlorine + Br - +I - ” assigned as group A, B and C respectively). Thirty HBPs were identified and 18 of them were never reported before. I - increases the transformation rate of BPA into HBPs as I-BPAs act as intermediate HBPs during chlorination that easily react with HClO/ClO - and HBrO/BrO - to form Cl-BPAs and Br-BPAs. HIO/IO - showed higher reactivity towards BPA and HBPs than that of HBrO/BrO - and HClO/ClO - . The recycling of I - was observed in the reactions of “BPA + chlorine + I - ” and “BPA + chlorine + Br - +I - ”, which may explain why I - can induce BPA to transform into HBPs and suggests that I - may act as a catalyst during the BPA chlorination reactions. The reaction pathways are proposed which present the reactions of BPA and HBPs with HClO/ClO - , HBrO/BrO - , and HIO/IO - , as well as the recycling of I - . This study describes the potential DBP formation and transformation mechanisms of BPA and its 16 alternatives, as well as the role of I - on the transformation of phenol compounds during chlorination.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2021
·
IF 2.694
Kuo Zhou,Xingfan Wang,Junfang Yang,Fenli Jin,Huan Zhou
The solubility equilibrium of Li+, Na+//Cl–, CO32– −H2O quaternary systems at 323.15 K and 348.15 K was studied via the isothermal solubility equilibrium method, and the complete phase diagrams were obtained including the properties of liquid density and pH. Solid species of LiCl·H2O, Li2CO3, NaCl, and Na2CO3·H2O are found in the quaternary system at 323.15 K and 348.15 K, and one double salt of Li2CO3·Na2CO3 is found at 348.15 K. The liquid phase of two invariant points and five univariant curves at 323.15 and three invariant points and seven univariant curves at 348.15 K in the quaternary system is determined. Li2CO3 covers the largest solid phase region and is hardly influenced by temperature; Li2CO3–NaCl is a stable salt pair, and its cosaturated solubility is the least at the diagonal line of Li2CO3–NaCl.
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CERAMICS INTERNATIONAL
·
2020
·
IF 3.83
Yanli Zhang,Zongchao Zhu,Yiheng Gu,Han Chen,Yifeng Zheng,Lin Ge
In this paper, a novel Cl − anion doping strategy is proposed to modify the electrochemical performance of Sr 2 Fe 1.5 Mo 0.5 O 6− δ (SFM) cathode for solid oxide fuel cells. A series of Cl-doped Sr 2 Fe 1.5 Mo 0.5 O 6− x − δ Cl x (SFMCl x , x = 0, 0.1, 0.2, 0.3, 0.4) materials is synthesized by the citric acid–glycine combustion method, and the effect of Cl doping on the crystal structure and electrochemical performance is systemically investigated. The doping of Cl into the SFM leads to the lattice expansion, and the electrochemical performance of Cl-doped SFMCl x cathodes is effectively improved as a result of the enhanced mobility of lattice oxygen introduced by Cl doping. The optimal composition with x = 0.2 (sample Sr 2 Fe 1.5 Mo 0.5 O 5.8− δ Cl 0.2 , noted as SFMCl0.2) exhibits a minimum polarization resistance R p value of 1.987 Ω cm 2 at 600 °C, reduced by 38.04% compared with the SFM cathode. These results suggest that Cl doping is an effective strategy to improve the electrochemical properties of cathode for solid oxide fuel cells.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Lin Cao,Jinming Piao,Wei Wang,Weijie Fan,Dongxiao Han,Yantong Pei,Ye Chen,Yue Zhang
To enhance corrosion resistance and extend the service life of coatings, layered double hydroxides (LDH) have been embedded into coatings to create a hybrid of organic–inorganic micro/nano-containers, improving the coatings’ physical barrier properties. Herein, an elaborately designed strategy is proposed to in-situ grow LDH on nanofibers , thereby obtaining polyvinylidene difluoride/hydrotalcite@deprotonated benzotriazole (PVDF/LDH@BTA − ) composite nanofibers , followed by incorporation into an epoxy resin to formulate the composite coating. The even distribution of LDH within the coating, aided by nanofibers, significantly bolstered the coating’s barrier effect. Upon exposure to corrosive environments, the hydrotalcite structure within PVDF/LDH@BTA − adsorbs chloride ions through anion exchange, capturing up to 0.26 mmol/cm 2 of chloride ions. Concurrently, corrosion inhibitors were released, forming a protective layer on the copper surface to substantially mitigate the corrosion process. This innovative approach markedly enhances the composite coating’s long-term corrosion resistance.
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JOURNAL OF POWER SOURCES
·
2017
·
IF 6.395
Bo Li,Yanan Zhang,Luyuan Zhang,Longwei Yin
Inorganic CsPbBr 3 perovskite is arousing great interest following after organic-inorganic hybrid halide perovskites, and is found as a good candidate for photovoltaic devices for its prominent photoelectric property and stability. Herein, we for the first time report on PbCl 2 -tuned inorganic Cl-doped CsPbBr 3 (Cl) perovskite solar cells with adjustable crystal structure and Cl doping for enhanced carrier lifetime, extraction rate and photovoltaic performance . The effect of PbCl 2 on the morphologies, structures, optical, and photovoltaic performance of CsPbBr 3 perovskite solar cells is investigated systemically. Compared with orthorhombic CsPbBr 3 , cubic CsPbBr 3 demonstrates a significant improvement for electron lifetime (from 6.7 ns to 12.3 ns) and diffusion length (from 69 nm to 197 nm), as well as the enhanced electron extraction rate from CsPbBr 3 to TiO 2 . More importantly, Cl doping benefits the further enhancement of carrier lifetime (14.3 ns) and diffusion length (208 nm). The Cl doped cubic CsPbBr 3 (Cl) perovskite solar cell exhibits a J sc of 8.47 mA cm −2 and a PCE of 6.21%, superior to that of pure orthorhombic CsPbBr 3 (6.22 mA cm −2 and 3.78%). The improvement of photovoltaic performance can be attributed to enhanced carrier lifetime, diffusion length and extraction rates, as well as suppressed nonradiative recombination.
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Small
·
2017
·Vol. 13
·期 23
·1700484
·
IF 8.643
Ning Zhou,Yiheng Shen,Yu Zhang,Ziqi Xu,Guanhaojie Zheng,Liang Li,Qi Chen,Huanping Zhou
Engineering the chemical composition of organic and inorganic hybrid perovskite materials is one of the most feasible methods to boost the efficiency of perovskite solar cells with improved device stability. Among the diverse hybrid perovskite family of ABX 3 , formamidinium (FA)-based mixed perovskite (e.g., FA 1− x Cs x PbI 3 ) possesses optimum bandgaps, superior optoelectronic property, as well as thermal- and photostability, which is proven to be the most promising candidate for advanced solar cell. Here, FA 0.9 Cs 0.1 PbI 3 (Cl) is implemented as the light-harvesting layer in planar devices, whereas a low temperature, two-step solution deposition method is employed for the first time in this materials system. This paper comprehensively exploits the role of Cs + in the FA 0.9 Cs 0.1 PbI 3 (Cl) perovskite that affects the precursor chemistry, film nucleation and grain growth, and defect property via pre-intercalation of CsI in the inorganic framework. In addition, the resultant FA 0.9 Cs 0.1 PbI 3 (Cl) films are demonstrated to exhibit an improved optoelectronic property with an elevated device power conversion efficiency (PCE) of 18.6%, as well as a stable phase with substantial enhancement in humidity and thermal stability, as compared to that of FAPbI 3 (Cl). The present method is able to be further extended to a more complicated (FA,MA,Cs)PbX 3 material system by delivering a PCE of 19.8%.
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