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Processes · 2022 ·Vol. 10 ·期 12 ·2562 · IF 3.352

Co-Precipitated Mn0.15Ce0.85O2−δ Catalysts for NO Oxidation: Manganese Precursors and Mn-Ce Interactions

Yuxi Gao,Baofang Jin,Xiaodong Wu,Zhenguo Li,Rui Ran,Duan Weng

Two Mn0.15Ce0.85O2−δmixed oxides were synthesized by a co-precipitation method using Mn(NO3)2and KMnO4as the manganese precursors, respectively. Structural analyses by X-ray powder diffraction and Raman spectroscopy reveal the formation of MnOx-CeO2solid solutions. The Mn0.15Ce0.85O2−δcatalyst prepared from the high-valent manganese precursor exhibits higher activity for the catalytic oxidation of NO. The advantage of KMnO4is related to the improved redox property of the catalyst as supported by H2temperature-programmed reduction (TPR) and O2temperature-programmed desorption (TPD). The Mn-Ce interactions create more Mn4+, Ce3+and oxygen vacancies on the KMnO4-synthesized mixed oxides based on the Raman and X-ray photoelectron spectra (XPS).Keywords:solid solutions;precursor;oxidation state;lattice defects;NO oxidation

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ENVIRONMENTAL POLLUTION · 2022 · IF 9.988

Highly efficient extraction of uranium from seawater by polyamide and amidoxime co-functionalized MXene

Di Zhang,Lijie Liu,Bing Zhao,Xiangxue Wang,Hongwei Pang,Shujun Yu

Uranium mainly exists in the form of uranyl carbonate in seawater. [UO 2 (CO 3 ) 3 ] 4- has strong stability, which increases the difficulty of uranium extraction from seawater. Meanwhile, the complex marine environment, a large number of coexisting competing ions and biological pollution are all non-negligible disturbing factors. Herein, we introduced amidoxime (AO) groups into the surface of Ti 3 C 2 and grafted polyamides (PA) by a simple one-step hydrothermal method to produce an efficient seawater uranium extraction adsorbent Ti 3 C 2 -AO-PA. Owing to the amidoxime groups, the material was highly selective for uranium. And the large number of amino groups in the polyamides gave it ideal resistance to biofouling. The possibility of Ti 3 C 2 -AO-PA as an adsorbent for uranium extraction from seawater was confirmed by various characterization techniques, numerous adsorption batch experiments, simulated seawater experiments and antibacterial performance tests. It was demonstrated that the uptake of [UO 2 (CO 3 ) 3 ] 4- by Ti 3 C 2 -AO-PA showed fast reaction kinetics (about 120 min), brilliant absorption capacity (81.1 mg·g −1 at pH 8.3), significant high selectivity (32.8 mg-U/g-Ads) and outstanding anti-biological contamination performance (92.9% antibacterial rate). XPS and DFT further indicated that the high extraction ability of Ti 3 C 2 -AO-PA for uranium was mainly attributed to the strong complexation of AO and –NH 2 with [UO 2 (CO 3 ) 3 ] 4- . These conclusions showed that Ti 3 C 2 -AO-PA not only had an ideal application prospect for uranium extraction from seawater, but also provided an available strategy for rapid and selective uranium adsorption from real seawater.

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Journal of Materials Research and Technology-JMR&T · 2023 · IF 6.4

Expanded graphite/Co@C composites with dual functions of corrosion resistance and microwave absorption

Shiqi Zhu,Yu Gao,Haoran Zhou,Chunlin Zheng,Xubin Li,Qikui Man,Xincai Liu

The development of microwave absorption materials with good environmental adaptability is a hot topic in the electromagnetic protection field. In this research, Expanded graphite (EG)/ZIF-67 nanocubes-derived (Co@C) composites were successfully fabricated by electrostatic assembly and subsequent heat treatment. The results show that the involvement of an appropriate content of Co@C not only overcomes the problem of single EG impedance mismatch but also introduces additional magnetic loss for the absorber. At the thicknesses of 1.6 mm and 1.5 mm, an effective absorption bandwidth (EAB) of 4.52 GHz and a minimum reflection loss (RL min ) of −48.4 dB were achieved for the Z2-700 sample with a low filling ratio (20 wt%). The enhancement of EMW-absorption performance is attributed to the optimization of impedance matching and the synergistic action between multiple loss mechanisms. Electrochemical corrosion test showed that graphite nanoflakes of EG enhanced the transfer resistance during corrosion, and the corrosion resistance of pure Co@C was enhanced with the protection of EG. This work provides a reasonable attempt to design and fabricate efficient microwave absorption materials suitable for harsh environments.

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Polymer Chemistry · 2023 ·Vol. 14 ·期 9 ·1043-1053 · IF 4.6

Conformational, crystalline and rheological properties of poly(octadecyl-co-methyl acrylate) statistically random copolymers

Xuejun Pan,Weiling Wu,Mo Zhu,Jixian Yang,Zhi-Chao Yan,Lianwei Li

This work reports the conformational, crystalline and rheological properties of poly(octadecyl-stat-methyl acrylate) (P(ODAx-stat-MAy)Nb) random copolymers, where Nb is the overall degree of polymerization, and x and y represent the molar fraction of ODA and MA, respectively, with x + y = 1.0. By a combination of ATRP, esterification and graft-onto strategies, a library of P(ODAx-stat-MAy)Nb samples with statistically random distribution features have been prepared. The average molar mass (M), viscometric radius (Rη) and intrinsic viscosity ([η]) are determined in solution, and a scaling-law of Rη ∼ M0.28 is established. For the conformation of P(ODAx-stat-MAy)Nb, it is found that [η] increases with x first due to chain expansion but decreases with x when x > 0.25, because the increase in segmental density dominates at high x. The rheological measurement indicates that the viscous flow activation energy remains constant first and then increases with decreasing x, reflecting the reduction of internal plasticization. In addition, the entanglement plateau modulus for the sample with x = 0.99 is one decade lower than that of the backbone, which is consistent with the prediction for the densely grafted bottlebrush polymers. This work provides a new strategy to synthesize model PODA-based random copolymers, and clarifies the change of the chain conformation, crystalline properties, and rheological behavior with the grafting density x, and this knowledge could be used to regulate the conformation and processing properties of comb/bottlebrush polymers by precisely designing the alkyl side chain's grafting density and length.

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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS · 2023 · IF 6

Co-pyrolysis of chitin with nitrogen carriers: Kinetics, product characterization and bio-oil analysis

Jia Liu,Shanjian Liu,An Zhao,Dongmei Bi,Di Yao,Ranran Kong

Considering the depletion of fossil fuels and the cumbersome traditional synthesis process of chemical compounds containing nitrogen, there is increased interest in direct production of nitrogenous compounds (bio-oil) from nitrogen-rich pyrolysis of biomass. In this study, a new strategy for the preparation of both nitrogen-rich bio-oil and biochar by co-pyrolysis of chitin and nitrogen carriers was proposed. Four different nitrogen carriers (urea, ammonium acetate , glutamate, and polyurethane) were selected and the thermal behavior of the mixtures as well as the synergistic competitive effects between the pyrolytic volatiles were characterized. Simultaneously, the properties of the co-pyrolysis products and the distribution of the main components in bio-oil were analyzed. The results showed that co-pyrolysis of chitin and nitrogen carriers had a synergistic effect. Glutamate had the most significant inhibitory effect on volatile gases, while only polyurethane promoted the release of volatile gases. Compared to the pyrolysis of chitin alone, the addition of urea, ammonium acetate and polyurethane effectively reduced the activation energy of the reaction. The addition of nitrogen carriers promoted the production of amines. Co-pyrolysis of urea and glutamate (40%) increased the content of nitrogenous compounds by 14.84% and 3.41%, respectively. However, the addition of ammonium acetate and polyurethane hindered the conversion of oxygenated compounds to nitrogen-containing compounds. In addition, the formation pathways of chitin pyrolysis and co-pyrolysis products were summarized. This work expanded the boundaries of high-value utilization of chitin.

CAS / MDL: 1398-61-4
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Facile synthesis of N-doping carbon-encapsulated metal catalyst for CO2 electroreduction to CO

Yu Liu,Zhichao Miao,Manfen Liang,Jie Zhang,Jinping Zhao,Leilei Xu,Jin Zhou,Shuping Zhuo

Electrocatalysis of CO 2 to CO is not only conducive to the artificial carbon cycle, but also green and efficient technology for producing chemicals. In consideration of the practical application, the novel strategy for large-scale preparation of catalyst has great potential to be developed. Herein, a facile one-step approach was developed for constructing a group of N -doping carbon-encapsulated metal catalysts (M@N C (M = Fe, Co, and Ni)) for CO 2 electroreduction to CO. In addition, the impact of metal on catalytic performance was detailedly researched. Specifically, the Ni@N C catalyst achieves an excessive CO Faraday efficiency (FE CO ) (>90 %) on a broad achievable potential window of − 0.67 V to − 0.97 V vs RHE in the H-type cell. The optimal catalyst attains a FE CO of 98 % at − 0.57 V vs RHE and an industrial-relevant current density of 430 mA cm −2 at − 1.07 V vs RHE in the flow cell. This work provides a facile way to fabricate catalyst on a large scale with preeminent performance for industrial CO 2 electroreduction to CO.

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JOURNAL OF THE AMERICAN CERAMIC SOCIETY · 2022 ·Vol. 106 ·期 4 ·2702-2715 · IF 4.186

Liquid-phase sintering of ZrO2-based nanocrystalline glass–ceramics achieved by multielement co-doping

Le Fu,Bohan Wang,Ying Deng,Guofu Xu,Jiwu Huang,Håkan Engqvist,Wei Xia

Liquid-phase sintering (LPS) is an effective pathway to assist the densification of ceramics. However, it has seldom been used to densify glass–ceramics. In the present study, a multielement co-doping strategy has been utilized to achieve LPS of a ZrO 2 –SiO 2 nanocrystalline glass–ceramic. Compared with undoped samples densified by solid-state sintering, doping of equimolar Al, Y, and Ca promoted the densification of the glass–ceramic at lower temperatures with a faster densification rate. Ternary doping enhanced coarsening of ZrO 2 nanocrystallites during sintering and annealing. The distribution of dopants was carefully observed with X-ray energy-dispersive spectrometry technique in scanning electron transmission microscopy mode. Results showed that the three dopants showed different distribution behaviors. After sintering, Y dopants were predominately distributed in ZrO 2 nanocrystallites, whereas parts of Al and Ca dopants were distributed in ZrO 2 nanocrystallites and part of them co-segregated at the ZrO 2 /SiO 2 heterointerfaces. Meanwhile, the segregation of Ca dopant at some intergranular films among ZrO 2 nanocrystallites was observed. Redistribution of dopants did not occur during annealing.

CAS / MDL: 23519-77-9
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Nature Nanotechnology · 2023 ·Vol. 18 ·期 3 ·299-306 · IF 38.3

Coverage-driven selectivity switch from ethylene to acetate in high-rate CO2/CO electrolysis

Wei Pengfei,Gao Dunfeng,Liu Tianfu,Li Hefei,Sang Jiaqi,Wang Chao,Cai Rui,Wang Guoxiong,Bao Xinhe

Tuning catalyst microenvironments by electrolytes and organic modifications is effective in improving CO 2 electrolysis performance. An alternative way is to use mixed CO/CO 2 feeds from incomplete industrial combustion of fossil fuels, but its effect on catalyst microenvironments has been poorly understood. Here we investigate CO/CO 2 co-electrolysis over CuO nanosheets in an alkaline membrane electrode assembly electrolyser. With increasing CO pressure in the feed, the major product gradually switches from ethylene to acetate, attributed to the increased CO coverage and local pH. Under optimized conditions, the Faradaic efficiency and partial current density of multicarbon products reach 90.0% and 3.1 A cm −2 , corresponding to a carbon selectivity of 100.0% and yield of 75.0%, outperforming thermocatalytic CO hydrogenation. The scale-up demonstration using an electrolyser stack achieves the highest ethylene formation rate of 457.5 ml min –1 at 150 A and acetate formation rate of 2.97 g min –1 at 250 A.

CAS / MDL: 1309-37-1 20344-49-4
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JOURNAL OF NANOBIOTECHNOLOGY · 2023 ·Vol. 21 ·期 1 ·1-15 · IF 10.2

Near-infrared light triggered in situ release of CO for enhanced therapy of glioblastoma

Ge Juan,Zuo Miaomiao,Wang Qirong,Li Zhen

Background Photodynamic therapy (PDT) features high biocompatibility and high spatiotemporal selectivity, showing a great potential in glioblastoma (GBM) treatment. However, its application was restricted by the poor therapeutic efficacy and side effect. Results In this study, a therapeutic nanoplatform (UCNPs@Ce6/3HBQ@CM) with combination of PDT and CO therapy was constructed, in which a photoCORM and a photosensitizer were loaded onto the surface of upconversion nanoparticles (UCNPs) functioning as photon transducer. Benefitting from NIR excitation and multicolor emission of UCNPs, the penetration depth of excitation light is enhanced and meanwhile simultaneous generation of CO and ROS in tumor site can be achieved. The as-prepared nanocomposite possessed an elevated therapeutic efficiency with the assistance of CO through influencing mitochondrial respiration and depleting ATP, accompanying with the reduced inflammatory responses. By wrapping a homologous cell membrane, the nanocomposite can target GBM and accumulate in the tumor site, affording a powerful tool for precise and efficient treatment of GBM. Conclusion This therapeutic nanoplatform UCNPs@Ce6/3HBQ@CM, which combines PDT and CO therapy enables precise and efficient treatment of refractory glioblastoma.

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Magnetochemistry · 2023 ·Vol. 9 ·期 2 ·47 · IF 2.7

Fine-Grained Tb3Al5O12 Transparent Ceramics Prepared by Co-Precipitation Synthesis and Two-Step Sintering

Lixuan Zhang,Xiaoying Li,Dianjun Hu,Mariya Dobrotvorska,Roman Yavetskiy,Zhengfa Dai,Tengfei Xie,Qiang Yuan,Haohong Chen,Qiang Liu,Jiang Li

In recent years, transparent terbium aluminum garnet (TAG) ceramics have attracted much attention for use in high-power Faraday isolators. Fine-grained ceramics usually possess better mechanical properties and accordingly better service performance. In this work, transparent TAG ceramics with fine grains were prepared using a two-step sintering procedure based on the low-temperature sintering process to suppress grain growth. The composition of TAG precursor and powders calcined at different temperatures was studied in detail. The microstructure and relative density of air pre-sintered TAG ceramics were studied to meet the requirements of hot isostatic pressing (HIP) post-treatment. Driven by the low pre-sintering temperature in air, the average grain sizes of the obtained TAG ceramics after HIP treatment are about 2.9–5.3 μm. The TAG ceramics (1.2 mm thick) pre-sintered at 1450 °C with HIP post-treatment at 1550 °C for 3 h under a 176 MPa Ar atmosphere possess the highest in-line transmittance of 80.3% at 1064 nm. The Verdet constant of the TAG ceramics at 632.8 nm is −180.5 rad·T−1·m−1at room temperature, which is about 1.3 times larger than that of the commercial Tb3Ga5O12single crystals.

CAS / MDL: 1066-33-7 7784-27-2
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FUEL PROCESSING TECHNOLOGY · 2023 · IF 7.5

Enhanced phenanthrene hydrogenation saturation performance of Ni-Co/NiAlOX catalysts and its catalytic mechanism

Yu Chen,Zemin Zhao,Ze Li,Jieying Jing,Wenying Li

Hydrogenation saturation of phenanthrene was an effective method to acquire high energy density fuels. It is essential to design highly active and stable hydrogenation saturated catalyst to realize the above reaction. Herein, series of Ni-Co/NiAlOx catalysts were synthesized by reducing at different temperatures. Activity evaluation showed that the catalysts reduced at 560 °C (Cat-560) possessed a phenanthrene conversion amount of 8.0 mmol·g -1 active component·h −1 and 98% perhydrophenanthrene selectivity after running 6 h under 300 °C, 5 MPa. Furthermore, it was found that Cat-560 presented superior specific activity (4.3 mmol·kg −1 ·s −1 ) and TOF (41.1 × 10 −3  s −1 ) for symmetric octahydrophenanthrene hydrogenation (the rate determining reaction), and its specific activity was 3 times as high as that of the catalysts reduced at 520 °C The excellent hydrogenation performance of Cat-560 could be attributed to its special geometric and electronic structure. Characterization indicated that the Ni 2+ in Ni-Co/NiAlO X catalyst was mainly located in the nickel aluminum spinel octahedral sites, which was beneficial to the reduction of Ni and the formation of smaller Ni particles. Moreover, it was explored that the Ni d charge density of Cat-560 catalyst was −0.12 e, which was suitable for the adsorption and activation of phenanthrene and symmetric octahydrophenanthrene.

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SCIENCE OF THE TOTAL ENVIRONMENT · 2023 · IF 9.8

Toxic effects of disinfection by-products on Pseudokirchneriella subcapitata and co-cultured algae community

Jinjie Li,Tielan Wang,Junzeng Xue

The widespread use of disinfectants in response to the COVID-19 pandemic may increase the concentration of disinfection by-products (DBPs) in surface water, posing ecological risks. This study assessed the acute toxicity of haloacetic acids and halophenols DBPs to Pseudokirchneriella subcapitata , and evaluated the impact of environmental concentrations of DBPs on co-cultured algae communities. The results showed that after exposure to disinfection by-products, the photosynthetic pigments of Pseudokirchneriella subcapitata were significantly reduced, and the MDA content and antioxidant enzyme activity were increased. The results of the ecological risk assessment showed that the RQ values of TBAA, 2,4-DBP, and 2,6-DBP were >0.1, with medium and high ecological risks. Despite this, the three DBPs with the highest risk values had little effect on the community structure of co-cultured algae. In contrast, the disinfection by-products with low ecological risk had a greater impact on the community structure and greatly promote the growth of cyanobacteria, which may cause new ecological risks. Therefore, not only high-risk disinfection by-products need to be paid attention to, but the impact of low-risk disinfection by-products cannot be ignored.

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