Frontiers of Chemical Science and Engineering
·
2022
·Vol. 16
·期 12
·1689-1699
·
IF 4.803
Li Wang,Li Wen-Ying,Wang Xing-Bao,Feng Jie
Radicals are important intermediates in direct coal liquefaction. Certain radicals can cause the cleavage of chemical bonds. At high temperatures, radical fragments can be produced by the splitting of large organic molecules, which can break strong chemical bonds through the induction pyrolysis of radicals. The reaction between the formation and annihilation of coal radical fragments and the effect of hydrogen-donor solvents on the radical fragments are discussed in lignite hydrogenolysis. Using the hydroxyl and ether bonds as indicators, the effects of different radicals on the cleavage of chemical bond were investigated employing density functional theory calculations and lignite hydrogenolysis experiments. Results showed that the adjustment of the coal radical fragments could be made by the addition of hydrogen-donor solvents. Results showed that the transition from coal radical fragment to H radical leads to the variation of product distribution. The synergistic mechanism of hydrogen supply and hydrogenolysis of hydrogen-donor solvent was proposed.
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Science China-Chemistry
·
2023
·Vol. 66
·期 2
·449-458
·
IF 9.6
Huang Yaoyao,Yuan Zhangyu,Yang Jia,Yin Shungao,Liang Aihui,Xie Gang,Feng Chuizheng,Zhou Zhisheng,Xue Qifan,Pan Yang,Huang Fei,Chen Yiwang
Passivating the interfacial defects and reducing the interfacial non-radiative recombination losses are the keys to improving the photovoltaic performance of three-dimensional (3D) perovskite solar cells (PVSCs). Stacking two dimensional (2D) perovskites on 3D perovskite is a promising method for interfacial treatment that improves the stability and efficiency of PVSCs. Herein, we developed conjugated fluorinated benzimidazolium cation (FBIm + ) which can be inserted between 3D perovskite and hole-transporting layer (HTL) to form 2D perovskite in situ. The 2D single crystal structures of (FBIm) 2 PbI 4 and (FBIm) 2 PbBr 4 were achieved and confirmed by single-crystal X-ray diffraction (XRD), while few single crystals of 2D perovskite based on imidazolium or benzimidazolium anchors have been reported. The 2D perovskite can passivate the interfacial defects, induce better crystallinity and orientation, conduct lower trap density and extend carrier lifetime. Furthermore, the energy level arrangement can be regulated by changing the counterion from iodide to bromide, which can efficiently improve the hole extraction and device performances. As a consequence, the best efficiency of 23.00% for FBImBr-incorporated devices was achieved, while only 20.72% for the control device. Meanwhile, the PVSCs modified by FBImBr displayed excellent environmental stability due to the constructed hydrophobic 2D perovskite layer which can effectively block moisture permeation. This work develops a new path to design novel conjugated organic passivants to form 2D/3D perovskite structures.
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RARE METALS
·
2023
·Vol. 43
·期 2
·692-701
·
IF 8.8
Lv Ying-Tong,Zhang Teng-Fei,Hu Zhao-Tong,Xia Guang-Lin,Huang Ze-Ya,Liu Zhen-Hua,Que Li-Hua,Yuan Cai-Ting,Guo Fang-Qin,Ichikawa Takayuki,Yu Xue-Bin
Garnet-type solid-state batteries (SSBs) are considered to be one of the most promising candidates to realize next-generation lithium metal batteries with high energy density and safety. However, the dendrite-induced short-circuit and the poor interfacial contact impeded the practical application. Herein, interface engineering to achieve low interfacial resistance without high temperature calcination was developed, which Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) was simply coated with complex hydride (Li 4 (BH 4 ) 3 I (3L1L)) in various mass ratios n (Li 4 (BH 4 ) 3 I)-(100− n )LLZTO (10 ≤ n ≤ 40). The interfacial conductivity increases by more than three orders of magnitude from 8.29 × 10 −6 S·cm −1 to 1.10 × 10 −2 S·cm −1 . Symmetric Li cells exhibit a high critical current density (CCD) of 4.0 mA·cm −2 and an excellent cycling stability for 200 h at 4.0 mA·cm −2 . SSBs with polymeric sulfur-polyacrylonitrile (SPAN) cathode achieve a high discharge capacity of 1149 mAh·g −1 with a capacity retention of 91% after 100 cycles (0.2 C). This attempt guides a simple yet efficient strategy for obtaining a stable Li/LLZTO interface, which would promote the development of solid-state batteries. Graphical abstract
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MONATSHEFTE FUR CHEMIE
·
2023
·Vol. 155
·期 1
·99-104
·
IF 1.8
Dong Wenwen,Gong Tengfei,Liu Chaoyang,Lin Jia,Jia Qiang,Chu Changhu
Apixaban is a highly potent, selective, and efficacious inhibitor of blood coagulation factor Xa. A practical and efficient process has been developed for the preparation of the key intermediate of apixaban. Starting from inexpensive 4-chloronitrobenzene and piperidine, an eight-step procedure for the intermediate has been developed. In this case, sodium chlorite is used twice to oxidize the piperidine cycle to the corresponding lactam under a CO 2 atmosphere, resulting in the construction of two lactams. Furthermore, most of these reactions are highly efficient and practical as they occur under mild conditions. Most of the intermediates can be obtained through simple slurry or recrystallization, and column chromatography purification is not necessary. Graphical abstract
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POLYMER BULLETIN
·
2024
·Vol. 81
·期 13
·11421-11457
·
IF 3.1
Shekhar Navin,Mondal Abhijit
Polylactic acid (PLA), a highly promising biodegradable biopolymer, has been extensively studied over the last two decades. The thermoplastic polyester PLA is bio-based, compostable, and eco-friendly. Its monomer, lactic acid, is fermented from renewable plant sources like starch and sugar. Therefore, PLA is regarded as a desirable substitute for conventional petroleum-based polymers. Because of its biocompatible and biodegradable properties, U.S. FDA (Food and Drug Administration) has approved PLA as a biomedical material. PLA has excellent mechanical, physical, structural, and thermal properties, making it suitable for various applications. However, PLA has limitations such as low impact toughness, hydrophobicity, and slow degradation rate at ambient temperatures. This can be improved by different modification methods, such as copolymerization, making composites or blends of PLA with other biodegradable polymers, or incorporating additives. This review presents information about the various methods of synthesis of PLA, its properties, and the environmental degradation of PLA. In addition, the different processing techniques of PLA are also reviewed. Lastly, the applications of PLA in sectors such as packaging, biomedical, agricultural, automotive, and textile are also discussed. Graphical Abstract
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Nano Research
·
2023
·Vol. 17
·期 5
·3684-3692
·
IF 9.9
Wu Wenbo,Zhu Jiaye,Tong Yun,Xiang Shuangfei,Chen Pengzuo
Regulating the electronic structure of Bi-based materials by alloying engineering is promising to promote the electrocatalytic activity, but it remains some challenges to be solved. In this study, a facile electrochemical co-deposition strategy is developed to synthesize the bimetallic Bi 9 Cu 1 alloy nanosheet on carbon cloth (Bi 9 Cu 1 /CC), which represents a novel self-supporting electrode for the electrocatalytic carbon dioxide (CO 2 ) reduction reaction (CO 2 RR). The Bi 9 Cu 1 /CC catalyst has achieved a remarkable catalytic performance with high Faradaic efficiencies (FE) of over 90% for formate at wide potentials from −0.7 to −1.2 V vs. reversible hydrogen electrode (RHE). Moreover, the reversible Zn-CO 2 battery can be driven by Bi 9 Cu 1 /CC cathode with a largest power density of 1.4 mW·cm −2 , and superior operating stability. The systematic characterizations and electrochemical results confirm that the improved catalytic active sites, the enhanced mass/charge transport and the optimal reaction kinetics of Bi nanosheet are realized for CO 2 RR by Cu alloying. In situ attenuated total reflection infrared (ATR-IR) result confirms the bimetallic Bi-Cu active sites prefer to follow the ⋆OCHO conversion pathway. The density functional theory (DFT) calculations suggest that the Cu alloying contributes to the increased density of states near the Fermi surface of Bi and the optimized adsorption of ⋆OCHO intermediates on the Bi sites, resulting in the excellent catalytic performance.
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Science China-Chemistry
·
2022
·Vol. 65
·期 4
·719-725
·
IF 10.138
Zhang Yanhui,Li Fuming,Yang Rong,Yang Yun,Zhang Fangfang,Yang Zhihua,Pan Shilie
The design and synthesis of new deep-ultraviolet (DUV) optical materials are important but challenging. It is well known that the polarizability anisotropy of linear [BO 2 ] − is larger than those of [BO 3 ] 3− and [BO 4 ] 5− , which is the better choice for exploring excellent optical materials. Here, we search for such crystals in borate systems based on the unusual fundamental structural unit [BO 2 ] − . By combining the linear [BO 2 ] − with the traditional triangular [BO 3 ] 3− and tetrahedral [BO 4 ] 5− units, a new mixed metal borate, Rb 5 Ba 2 (B 10 O 17 ) 2 (BO 2 ) was obtained via high-temperature solution method. It exhibits excellent optical properties including a DUV transmission window (188 nm) and suitable birefringence (0.06). It also has good thermal stability and its crystal plates can be prepared easily. Furthermore, the strategies of designing borates with [BO 2 ] − units have been proposed from the transformation of crystal framework and the preparation method.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 60
·90248-90258
·
IF 5.19
Zhang Qian,Zhou Jinwen,Zhang Lishan,Zhong Shan,Ru Xuan,Shu Xiaohua
Pyrite affects the adsorption of tylosin (TYL) due to their coexistence in the lake system. As well as the reactivity groups of S–S-H, S-OH, and Fe-OH, defects also have the possibilities to influence the adsorption of organic contaminants. However, the role of these active sites in antibiotic adsorption on pyrite has not been deeply studied. Besides, pH, N, P, dissolved oxygen, and dissolved organic matter (DOM) fluctuate greatly in lake at different seasons, which may change the surface characteristics of pyrite. Hence, the adsorption of TYL on natural pyrite considered solution chemistry and DOM in lake water was explored in this study. The fitting results of the kinetic and isotherm models showed that the adsorption included physical and chemical interactions. The neutral initial solution pH was conductive to TYL adsorption owing to the combined result of electrostatic and cover of Fe-oxyhydroxide. NO 3 − and NH 4 + had no effect on TYL adsorption, whereas H 2 PO 4 − promoted adsorption by forming flocculent Fe(H 2 PO 4 ) 3 precipitates. The dissolved oxygen increased adsorption. This is due to the co-promotion of the pyrite oxidation by oxygen and sulfur defects. The Fe(II)-DOM complex caused by pyrite surface oxidation reduced the concentration of TYL in solution by gathering. Except for the surface charge, reactivity groups on pyrite significantly influenced the adsorption of TYL. The bond fracture of S–S resulted in sulfur defects that contributed to pyrite oxidation. As a result, Fe(III)/Fe(II) on the surface of pyrite or in solution produced a complex Fe(III)/Fe(II) with anions and DOM. In addition, Fe(III)-S on sulfur defects interacted with the O–H of TYL through hydrogen bonding. Furthermore, the Fe–O-C bond is formed by the interaction of C–OH on TYL and Fe(III) (hydr)oxides on the surface of pyrite. The study provides a deep insight into the effect of pyrite surface active sites on amphoteric antibiotic adsorption. It helps to understand antibiotic migration and interactions with widespread pyrite in the real environment. Graphical abstract
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HISTORICAL ARCHAEOLOGY
·
2024
·
IF 0.4
Ryzewski Krysta
Hamtramck, a small, century-old city completely enveloped by Detroit, is promoted by its leadership as “the world in 2.1 square miles.” This slogan invokes two inextricable facets of the city’s heritage and contemporary identity: Hamtramck’s longstanding reputation as a proud, working-class city that has always been welcoming to immigrants, and its significance as the former home of automotive manufacturer Dodge Main, whose operations between 1910 and 1979 positioned the city as a global industrial powerhouse. The Old Hamtramck Center Project combines historical, archaeological, and geospatial sources of data to examine the process of urban expansion in the new city, which included the dissonant relationships among local communities and the built environment. Archaeological investigations within Old Hamtramck Center consider how the city’s residents experienced the often inconsistent circumstances of rapid urbanization and civic organization as the rural village transformed into a crowded industrial city during the early 20th century.
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RARE METALS
·
2024
·
IF 9.6
Liu Ke-Xin,Tan Ran,Zheng Zhong,Zhao Rui-Rui,Ülgüt Burak,Ai Xin-Ping,Qian Jiang-Feng
Lithium metal, with its exceptionally high theoretical capacity, emerges as the optimal anode choice for high-energy-density rechargeable batteries. Nevertheless, the practical application of lithium metal batteries (LMBs) is constrained by issues such as lithium dendrite growth and low Coulombic efficiency (CE). Herein, a roll-to-roll approach is adopted to prepare meter-scale, lithiophilic Sn-modified Cu mesh (Sn@Cu mesh) as the current collector for long-cycle lithium metal batteries. The two-dimensional (2D) nucleation mechanism on Sn@Cu mesh electrodes promotes a uniform Li flux, facilitating the deposition of Li metal in a large granular morphology. Simultaneously, experimental and computational analyses revealed that the distribution of the electric field in the Cu mesh skeleton induces Li inward growth, thereby generating a uniform, dense composite Li anode. Moreover, the Sn@Cu mesh-Li symmetrical cell demonstrates stable cycling for over 2000 h with an ultra-low 10 mV voltage polarization. In Li||Cu half-cells, the Sn@Cu mesh electrode demonstrates stable cycling for 100 cycles at a high areal capacity of 5 mAh·cm −2 , achieving a CE of 99.2%. This study introduces a simple and large-scale approach for the production of lithiophilic three-dimensional (3D) current collectors, providing more possibilities for the scalable application of Li metal batteries. Graphical abstract
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2022
·Vol. 33
·期 13
·10611-10625
·
IF 2.779
Qu Mengnan,Sun Wenchao,Xue Yuyu,Pang Yajie,Shi Fan,Luo Zhanxia,Wang Rong,Peng Lei,He Jinmei
Cellulose and its derivatives are biopolymers abundant in nature, with the advantages of low cost, biodegradability, and high positive friction polarity. In this paper, a novel friction positive layer material sodium carboxymethyl cellulose (CMC)-epichlorohydrin (ECH)-polyethyleneimine (PEI) aerogel (CEP aerogel) and polytetrafluoroethylene (PTFE) film are reported as a friction pair to prepare high-performance CEP aerogel based triboelectric nanogenerator (CEP-TENG) for mechanical energy harvesting and sensing fields. The systematic optimization of the preparation process of CEP aerogel to improve its friction positive polarity not only expands the field of friction positive layer materials but also facilitates its better application to TENG with excellent output performance. The corresponding CEP-TENG can produce open-circuit voltage of 203 V, short-current density of 8.2 µA/cm 2 , and a power density of 3.38 W/m 2 under the applied force of 15 N and frequency of 4 Hz, which is 13.5 times and 27.3 times higher than that of CMC aerogel and 0.03 mm PTFE film. In addition, CEP aerogel-based TENGs have been proven to be effective in powering electronic devices by charging commercial capacitors and detecting human motion such as finger tapping and arm bends. Therefore, the investigation demonstrates the feasibility of CEP aerogel as a friction layer material, thus providing insights to promote low cost-effective and environmentally friendly TENG development.
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 12
·1-11
·
IF 5.833
Wang Xiao,Liao Xiaochen,Zhang Bingjian,Zhang Mengmeng,Mei Lisha,Wang Fangwai,Chen Siyu,Qiao Xiuwen,Hong Chenglin
Abstract Carcinoembryonic antigen levels in the human body reflect the conditions associated with a variety of tumors and can be used for the identification, development, monitoring, and prognosis of lung cancer, colorectal cancer, and breast cancer. In this study, an amperometric immunosensor with CuCo/carbon nanocubes (CuCo/CNC) as the signal label is constructed. The bimetal-doped carbon skeleton structure has a high specific surface area and exhibits good electrocatalytic activity. In addition, Au/g-C 3 N 4 nanosheets (Au/g-C 3 N 4 NSs) are used to modify the substrate platform, facilitating the loading of more capture antibodies. The reaction mechanism was explored through electrochemical methods, X-ray powder diffraction, X-ray photoelectron spectroscopy, and other methods. Kinetic studies have shown that CuCo/CNC have good peroxidase-like activity. In addition, the electrocatalytic reduction ability of CuCo/CNC on hydrogen peroxide can be monitored using amperometric i – t curve (− 0.2 V, vs. SCE), and the response current value is positively correlated with the CEA antigen concentration. The prepared electrochemical immunosensor has good selectivity, precision, and stability. The dynamic range of the sensor was 0.0001–80 ng/mL, and the detection limit was 0.031 pg/mL. In addition, the recovery and relative standard deviation in real serum samples were 97.7–103 % and 3.25–4.13 %, respectively. The results show that the sensor has good analytical capabilities and can provide a new method for the clinical monitoring of CEA. Graphic abstract
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