GREEN CHEMISTRY
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2022
·Vol. 24
·期 3
·1362-1372
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IF 11.034
Weisheng Yang,Juan Wang,Liang Jiao,Yang Song,Chang Li,Chaoquan Hu
Common technologies for waste polyethylene terephthalate (PET) hydrolysis generally use strong acids or alkalis as catalysts; however, these processes are costly and generate a large amount of acid, alkali, and salt wastewater. In addition, these catalysts are difficult to recycle and reuse, which is not in line with the concept of sustainable development. This study describes the use of concentrated p-toluenesulfonic acid (PTSA) as an acid catalyst for PET hydrolysis under relatively mild conditions, enabling the degradation of approximately 100% of PET into 96.2% of terephthalic acid (TPA) within 90 minutes at 150 °C. A similar degradation efficiency can only be achieved at 150 °C using concentrated sulfuric acid for over 5 h. The generated TPA was easily separated from the hydrolysis system via filtration. The used PTSA was easily recovered from the filtrate after TPA collection using simple concentration and crystallization technologies. The recovered PTSA still maintained excellent catalytic efficiency for PET hydrolysis after five consecutive cycles. Furthermore, the kinetics of the reaction confirmed that the PET hydrolysis catalyzed by concentrated PTSA conforms to a first-order reaction with a relatively low apparent activation energy of 76.4–125.4 kJ mol−1. Finally, the technical feasibility and environmental impact of a scale-up were evaluated using Aspen Plus simulations. Overall, this work proposes a feasible and green strategy for the low-cost and environmentally friendly hydrolysis of waste PET.
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POLYMER DEGRADATION AND STABILITY
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2022
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IF 5.204
Wentao He,Huahui Xu,Pingan Song,Yushu Xiang,Shuhao Qin
Flame-retardant functionalized nanomaterials have attracted much research interests due to the combined advantages of organic and inorganic components. In the present study, P, N-decorated halloysite nanotube (MA-PPA@HNT) was prepared via simple steps of phenphosphinic acid intercalation and subsequent electrostatic interaction with melamine. Compared to unmodified HNT, the incorporation of MA-PPA@HNT into polyamide 6 (PA6)/aluminum diethylphosphinic acid (AlPi) composite results in significant improvement of flame retardancy. At equal HNT loading of 2wt%, the UL-94 rating grade of PA6/AlPi/MA-PPA@HNT composite was V-0, whereas that of PA6/AlPi/HNT composite V-2. And compared with PA6 , there is a decrease of peak heat release rate (pHRR) and total heat release (THR) by 72.6% and 17.4%, respectively. The flame retardant mechanism was analyzed by cone calorimetry, gas volatility and characterization of char residues. It is considered that MA-PPA@HNT plays the critical role of promoting the formation of P, Si-rich intumescent char in the condensed phase and enhancing the barrier effect for heat and mass transfer.
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ACS Catalysis
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2022
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IF 13.7
Yuqin Chen,Yameng Zhu,Huixiang Sheng,Jin Wang,Chengyu Zhang,Yaqi Chen,Wei Huang,Gang Lu
Surface plasmons have received much attention in chemical reactions because of their high light-utilizing efficiency, high reaction rate, and mild reaction conditions. However, the potential of plasmonic photochemistry has not been fully exploited, mainly due to the limited lifetime of plasmon-generated hot carriers. Herein, using in situ Raman spectroscopy, we reveal that the coadsorption of p-hydroxythiophenol (PHTP) molecules significantly accelerates the plasmon-mediated decarboxylation reaction of p-mercaptobenzoic acid adsorbed on silver nanoparticles. The observed boosting of the decarboxylation reaction is attributed to the matched energy distribution of the plasmon-generated hot electrons to the lowest unoccupied molecular orbital (LUMO) level of the coadsorbed PHTP molecules. Our findings will help not only to deepen the understanding of the plasmon-mediated chemical reactions but also to fabricate highly efficient plasmonic catalysts conveniently and cost-effectively.
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CRYSTENGCOMM
·
2022
·Vol. 24
·期 40
·7200-7215
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IF 3.756
Ningjing Song,Jiangfeng Li,Baosheng Li,Ercai Pan,Juan Gao,Yurong Ma
The shells of P. placenta are composed of foliated calcite laths packed as layered structures and have high mechanical properties and optical transparency. However, the biomineralization mechanism and the influence of the organic matrix on the formation of the foliated calcite laths in the shells of P. placenta are not known. The acid-soluble matrix (ASM) was extracted from the shells of P. placenta and characterized in detail. Sixteen proteins including calcium-binding and chitin-binding proteins were associated to shell formation via proteome analysis of ASM. The ASM was found to be enriched with Gly, Asp and Ser. By tracking the Ca2+ concentration in the solution in the presence of ASM by a potentiometric method, we find that the ASM has a strong effect to stabilize the amorphous calcium carbonate (ACC) precursor in solution with a nucleation time of about 7733 s and a retardation factor of about 2.3, while the concentration of the ASM was 0.3 μg mL−1. In particular, the ASM can inhibit the (secondary) nucleation of calcium carbonate for 10 and 24 hours on the shell surfaces of P. placenta and the glass substrate in the aqueous solution, respectively. An explosive secondary nucleation and quick crystal growth from 50 nm to 10 μm can be finished on the shell surfaces in one hour, in between 10 h and 11 h of reaction time, via a gas diffusion process. This indicates that the ASM has a very strong effect to stabilize ACC and inhibit nucleation. The formation of ACC in the solution and its transformation to calcite crystals on the substrates were tracked by dynamic light scattering, selected-area electron diffraction, infrared spectroscopy, scanning electron microscopy, and confocal laser scanning microscopy. It was found that the ASM was doped in the preliminary nanocrystals with a size of about 50–100 nm, which were formed on the shell surfaces via secondary nucleation, and was occluded into the calcite crystals without preferred adsorption on particular crystal planes. The calcite crystals formed on the shell surfaces became more and more rounded and lost {104} planes with increasing concentration of the ASM in the solution, indicating that the ASM can stabilize other planes instead of the thermodynamic {104} planes. The in vitro crystallization study in this work shows that ASM extracted from the shells of P. placenta has a strong effect on the biomineralization process of foliated calcite laths of P. placenta.
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
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2022
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IF 4.383
Cheng Wang,Jiale Yu,Kai Feng,Huidong Guo,Lipeng Wang
In this study, natural clinoptilolite was treated with NaOH solutions of different concentrations under mild ambient conditions. The composition and structure of the as-prepared samples were characterized, and their performance was assessed in terms of the removal of the heavy metal ions Cd 2+ , Cu 2+ , and Cr 3+ from the aqueous solution. The results showed that the composition, structure, and capability of removal of heavy metal ions of the samples were significantly influenced by the NaOH concentrations. The crystal structure of clinoptilolite remained invariant under a relatively low NaOH concentration (≤0.5 M), began transforming into zeolite Na–P under a medium NaOH concentration (∼1.0 M), and then completely transformed into it under a high NaOH concentration (2.0–4.0 M). The samples treated with NaOH had lower SiO 2 /Al 2 O 3 ratios, and were superior to unmodified natural zeolite in removing the heavy metal ions. This method of treatment with relatively high concentrations of NaOH is a simple and effective way to transform natural clinoptilolite into the zeolite Na-P rich ion exchanger, which is suitable for removing heavy metal ions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Xinxin Han,Bingjie Lu,Xin Huang,Cheng Liu,Shixia Chen,Jingwen Chen,Zheling Zeng,Shuguang Deng,Jun Wang
S-scheme photocatalysts are more efficient than the conventional type-II configuration, but the CO 2 reduction performances are still unsatisfactory. Herein, we firstly report the layered double hydroxide (LDH) based S-scheme heterostructure photocatalyst (NiIn LDH/In 2 S 3 ) with n-type NiIn LDH and p-type In 2 S 3 . The built-in internal electric field directs the photogenerated electrons flow from the conductive band of In 2 S 3 to the valance band of NiIn LDH, which is confirmed by operando and theoretical experiments. The CO 2 photoreduction intermediates are monitored by in-situ Raman spectra, and the density functional calculations disclose the reduced energy barrier for CO desorption on the heterojunction. Therefore, without cocatalysts or sacrificial agents, the NiIn LDH/In 2 S 3 heterojunction delivers a high CO yield rate of 29.43 μmol g −1 h −1 under visible light irradiation, ca. 3.5 and 4.3 times higher than the single counterpart NiIn LDH and In 2 S 3 . Notably, this value is the highest among S-scheme CO 2 photocatalysts and surpasses most top-ranking benchmarks.
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ACS Applied Energy Materials
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2021
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IF 6.024
Shuyao Li,Junhua Jiang,Zheng Ma,Yanqun Chen,Lanwei Li,Jianli Wang,Chao Wang
As we all know, the introduction of porous structure into the matrix is a very effective method to enhance the material’s thermoelectric performance. Herein, Er-doped Bi0.46Sb1.54Te3 bulk materials were successfully synthesized by high-energy ball milling and spark plasma sintering. The carrier mobility is enhanced and the carrier concentration is optimized by Er doping, thereby improving the electrical transport properties. Furthermore, the dispersed secondary phase nanoparticles and pores introduced by Er doping provide additional phonon scattering, which leads to the decreased lattice thermal conductivity. Finally, the Erx(Bi0.23Sb0.77)2–xTe3 (x = 0.02) sample shows a maximum ZT value of 1.21 at 350 K, and the average ZT value of 1.17 between 300–400 K is achieved.
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ACS Applied Materials & Interfaces
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2021
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IF 9.229
Chunyan Wang,Jihuai Wu,Shibo Wang,Xuping Liu,Xiaobing Wang,Zhongliang Yan,Liqiang Chen,Xiao Liu,Guodong Li,Weihai Sun,Zhang Lan
The practical applications of perovskite solar cells (PSCs) are limited by further improvement of their stability and performance. Additive engineering and interface engineering are promising medicine to cure this stubborn disease. Herein, an alkali metal fluoride as an additive is introduced into the tin oxide (SnO2) electron transport layer (ETL). The formation of coordination bonds of F– ions with the oxygen vacancy of Sn4+ ions decreases the trap-state density and improves the electron mobility; the hydrogen bond interaction between the F ion and amine group (FA+) of perovskite inhibits the diffusion of organic cations and promotes perovskite (PVK) stability. Meanwhile, the alkali metal ions (K+, Rb+, and Cs+) permeated into PVK fill the organic cation vacancies and ameliorate the crystal quality of PVK films. Consequently, a SnO2-based planar PSC exhibits a power conversion efficiency (PCE) of 20.24%, while the PSC modified by CsF achieves a PCE of 22.51%, accompanied by effective enhancement of stability and negligible hysteresis. The research results provide a typical example for low-cost and multifunctional additives in high-performance PSCs.
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PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Jiayi Li,Ying Huang,Minhua Su,Yuying Xie,Diyun Chen
Heterocyclic aromatic compounds such as malachite green can cause immense harm to the environment and mankind because of their toxic bio-accumulation and insufficient biodegradation. ZnFe 2 O 4 /TiO 2 (ZF-T) has attracted attentions as a visible-light-driven catalyst because it can break and mineralize benzene through photolysis. Compared with TiO 2 , which photodegrades only 53.5% malachite green, anatase TiO 2 loaded with ZnFe 2 O 4 has greater photocatalytic activity and can degrade up to 90.1% malachite green. Furthermore, a photocatalytic efficiency above 80% can be obtained through five consecutive cycles with a duration of 4 h. In this study, ZF-T was characterized, and its photolytic parameters, including dosage, pH, time, and ionic strength, were optimized. The photolytic products of malachite green were analyzed by ultraviolet–visible spectroscopy and liquid chromatography-mass spectrometry, which confirmed that ZF-T can drive visible light to produce •O 2 − and H + free radicals that can efficiently degrade heterocyclic aromatic hydrocarbons and cleave benzene rings. These outcomes deepen our understanding of the development and applications of visible-light-driven ZF-T composites in the field of wastewater purification.
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SOLAR ENERGY
·
2021
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IF 5.742
Yujiao Li,Pin Lv,Chen Li,Fan Xu,Jinbiao Jia,Bingqiang Cao
Traditional P-i-N perovskite solar cells have achieved high efficiency over 25%, but the device structure is relatively complex, and generally requires expensive low-conductivity p-type organic semiconductors as hole transport materials. As a typical semiconductor, it is very important to realize the bipolar doping of methylamine lead iodine (CH 3 NH 3 PbI 3 ) that is the light-absorbing layer of perovskite solar cell. Also, it is significant to develop perovskite cells with new device structure. Here, we chose lithium iodide (LiI) as the dopant and successfully grow p-type Li + doped CH 3 NH 3 PbI 3 (MAPbI 3 :Li) perovskite films with low resistivity (10 3 Ω•cm). The temperature-dependent photoluminescence, Hall effect and Kelvin probe force microscope (KPFM) results strongly confirmed that Li + doping promotes the transformation of pristine weak n-type MAPbI 3 to intentionally doped p-type film. Subsequently, the p-type MAPbI 3 film is used as both the light absorption layer and hole transport layer, and form a PN heterojunction with n-type titanium dioxide (TiO 2 ), which is used as the electron transport layer, to construct the heterostructural perovskite cell with a photoelectric conversion efficiency (PCE) of 10.43%. The electron beam induced current (EBIC) signal also strongly confirms the existence of the PN heterojunction and the new working mechanism of such new solar cells.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Yong Wang,Shouzhu Li,Dafeng Zhang,Fang Tan,Lei Li,Guangzhi Hu
Highly efficient electrocatalysts with low cost for electrochemical water splitting is important for the intermediate energy conversion. In the present work, P and Cu dual-doped cobalt selenide nanoarrays with hierarchical structure were fabricated via a facile hydrothermal method, involving in-situ growth on a self-supported conductive Ni foam substrate (P,Cu-Co 0.85 Se/NF). The overall water splitting (OWS) performance of the catalysts was systematically studied in alkaline solution. Compared to single-ion-doped or pure Co 0.85 Se, dual incorporation of the anion and cation can contort the lattice and induce powerful electronic interactions, thereby exposing abundant catalytic sites and optimizing the adsorption energy of the reaction intermediates. Benefiting from the merits of P, the Cu-co-doped Co 0.85 Se/NF electrode exhibited outstanding catalytic activity towards hydrogen evolution reaction (HER), generating a 10 mA cm −2 current density at the overpotential of 96.8 mV in 1 M KOH, and the overpotential is 300 mV towards oxygen evolution reaction (OER) with the current density of 100 mA cm −2 . Furthermore, when applied it to fabricate OWS cell, the cell voltage is as low as 1.57 V at the current density of 10 mA cm −2 . This present work broaden the potential application of the electrocatalytic performance of transition metal dichalcogenides .
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OPTICAL MATERIALS
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2021
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IF 3.08
Xue Li,Li-Juan Jian,Li Wang,Rong-Han Liu,Yun Zhao,Jiang-Tao Chen,Yan Li
Strategy of designing new-structured semiconductor photocatalysts with great electron-hole pairs separation is meaningful for improving the photocatalytic pollution abatement. Herein, on the basis of decahedral BiVO 4 with largely exposed (040) crystal facet, p-n hetero-nanostructured NiS@(040)-BiVO 4 catalysts with various molar ratio of NiS were fabricated by a facile two-step hydrothermal method to study the photo-degradation activities under visible-light irradiation. To photo-degrade anion methyl orange (MO), cation rhodamine B (RhB) and tetracyclines (TC), such nanostructures can all exhibit excellent photocatalytic activities . Compared with pure (040)-BiVO 4 and NiS nanoparticles , 0.6 M ratio of NiS@(040)-BiVO 4 possesses 8.6, 8.9 and 6.5 times higher photocatalytic capacity (MO: 98.6%, RhB: 99.1%, TC: 98.4%) and 49.2, 64.2 and 27.7 times faster photocatalytic rate (MO: 8.4060 h −1 , RhB: 8.2854 h −1 , TC: 7.6230 h −1 ). Detailed analyses show the superior light-harvesting, higher photocurrent response, excellent charge separation and improved charge transport properties are the main factors resulting the high efficient photocatalytic performance of NiS@(040)-BiVO 4 nanostructures. Besides, the forming of facet isotype heterojunctions between (040) and (220) lattice planes in BiVO 4 can also help to get more active photo-induced electrons for photocatalysis .
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