DYES AND PIGMENTS
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2022
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IF 5.122
Juan Fu,Ziyang He,Xin Hu,Teng Guo,Ye Liang,Fengjie Deng,Meiying Liu,Yuanqing Wen,Xiaoyong Zhang,Yen Wei
Fluorescent materials with aggregation-induced emission (AIE) have standout as one of the most interesting candidates for biomedical applications. The development of new methods for fabrication of AIE-active materials will surely advance their applications in related fields. In this work, we reported a novel method for preparation of AIE-active luminescent polymer (Lys-PEG-TPE) through a three-component reaction involving carbon dioxide (CO 2 ) using lysine, Polyethylene glycol (PEG) and AIEgen as the reactants. On account of the introduction of PEG , Lys-PEG-TPE could well disperse in aqueous solution, while hydrophobic TPE will aggregate in the core of self-assembled nanoparticles , endowing the obvious enhancement of fluorescence intensity. Results from biological assays suggested that Lys-PEG-TPE exhibits almost no toxicity after incubation with HepG2 cells and its fluorescence can be clearly observed in cytoplasm after cell internalization. More importantly, the AIE feature of Lys-PEG-TPE could not only effectively solve the aggregation-induced quenching effect of traditional fluorescent molecules, the carboxyl groups of lysine could also be used for loading functional cationic ions (e.g., anticancer drugs or imaging agents) to fabricate multifunctional theranostic and imaging composites. Considering the benign reaction conditions, high atom economy, and well tunability of reactants of multicomponent reactions, this strategy should be of broad interesting for fabrication of multifunctional AIE-active materials for biomedical applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Tengfei Zhang,Peng Zheng,Fangna Gu,Wenqing Xu,Wenxing Chen,Tingyu Zhu,Yi-Fan Han,Guangwen Xu,Ziyi Zhong,Fabing Su
Hydrogenation of CO 2 into CH 4 is an effective strategy for dealing with CO 2 -relevant environmental problems. Since the CO 2 methanation reaction involves multiple electron transfers and various C1 intermediates, improving the reaction rate at each step is critical to accelerating the entire reaction. Here, we report a dual-active-site tandem catalyst (Ru 1 Ni/CeO 2 ) composed of Ru single atoms (Ru 1 ) and Ni nanoparticles , which can effectively convert CO 2 to CH 4 , showing ∼90% CO 2 conversion and ∼99% CH 4 selectivity at 325 °C, much higher than those of the Ru 1 /CeO 2 and Ni/CeO 2 catalysts. Experimental and theoretical calculation results reveal that Ru 1 is extremely active for converting CO 2 to CO, while the Ni site is highly efficient for the subsequent sequential CO to CH 4 reaction step. The coexistence of the Ru 1 and Ni sites significantly boosts the overall reaction. This work offers a promising strategy for the rational design of efficient multisite tandem catalysts.
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APPLIED SURFACE SCIENCE
·
2022
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IF 7.392
Fangfang Cai,Xia Hu,Faliang Gou,Yuyuan Chen,Yulu Xu,Chenze Qi,De-Kun Ma
Ternary ZnIn 2 S 4 (ZIS) is a kind of potential electrocatalyst for CO 2 reduction reaction (CO 2 RR). However, the reported reduction products are usual C1 species. Considering that N doped carbon can increase adsorption of CO 2 molecules, facilitate electron transfer, and activate active sites, here ultrathin ZIS nanosheet arrays (ZIS NSAs) grown on N doped carbon cloth (NDCC) were synthesized through a facile hydrothermal route. The as-synthesized ZIS NSAs/NDCC enabled electrocatalytic CO 2 RR toward ethanol with the highest 42 % faradaic efficiency (FE) at an applied potential of − 0.7 V versus the reversible hydrogen electrode (RHE) in CO 2 -saturated 0.5 M KHCO 3 aqueous solution. This is first report on ZIS-based electrocatalyst for electrocatalytic CO 2 RR toward ethanol production. The experimental results and density functional theory (DFT) calculations showed that NDCC could enhance the CO 2 RR activity and promote CO-CO coupling process. Our work not only provides a new electrocatalyst for CO 2 RR to ethanol but also stresses the influence of N doped carbon substrate and bimetallic effect on electrocatalytic CO 2 RR.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Jialin Wu,Xuan Liu,Rumeng Zhang,Jianbin Zhang,Huayan Si,Zhaojun Wu
A simultaneous titration-calcination strategy was proposed to synthesize core–shell type (CaCO 3 /Ce(OH)CO 3 )@Ce(OH)CO 3 precursors by titrating Ca 2+ and Ce 3+ into aqueous CO 2 storage material (CO 2 SM) solution simultaneously without adding any templating agents or surfactants. After calcination at 900 °C, the novel core–shell type (CaO/CeO 2 )@CeO 2 composite adsorbent with the strong stability of adsorption cycle was synthesized. The effects of Ca/Ce doping ratio, CO 2 SM dosage, drop rate and temperature conditions on the CO 2 adsorption performance on the composite adsorbent during the calcium cycle were investigated. The synthetic adsorbent with a Ca/Ce doping ratio of 24: 1 had the strongest CO 2 capture performance during the calcium cycle, and it mainly consisted of CaO and CeO 2 . The CO 2 adsorption amount still maintained at about 430 mg/g after 15 cycles under the adsorption–desorption conditions at 750 °C and 900 °C. (CaO/CeO 2 )@CeO 2 composite adsorbent is a core–shell structure with CeO 2 as the shell and CaO/CeO 2 as the liner, in which CeO 2 is uniformly dispersed in CaO pore channels, which gives the adsorbent a stable pore structure and enhances the anti-sintering performance of Ca-based adsorbent. Due to the special property of CeO 2 , it can also promote the ion migration during the carbonation process, thus maintaining the adsorption activity. Density functional theory (DFT) calculations successfully explain why CeO 2 can be used as an inert dopant to promote the adsorption of CO 2 . After that, the synthesis mechanism of core–shell adsorbent and the reaction mechanism of CO 2 adsorption are proposed in conjunction with the series characterization. This work provides a new strategy for the efficient synthesis of Ca-based adsorbents with special morphology and a new idea for CO 2 capture.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Pengxin Zeng,Chuanwen Zhao,Chenxi Liang,Peiyu Li,Haoxuan Zhang,Ruilin Wang,Yafei Guo,Hongqiang Xia,Jian Sun
K 2 CO 3 -based adsorbent pellets produced by graphite-casting method are promising alkali metal-based solid CO 2 adsorbents. The incorporation of porous metal oxide supports is an effective to enhance CO 2 adsorption capacity of K 2 CO 3 -based adsorbent pellets. In this work, graphite-casted K 2 CO 3 -based adsorbent pellets incorporated with different porous supports (i.e., TiO 2 , ZrO 2 , and SiO 2 ) were prepared for CO 2 capture. Comparatively, the ZrO 2 -supported, K 2 CO 3 pellets loaded with 30 wt% of K 2 CO 3 exhibit the highest CO 2 adsorption capacity, approximately 0.93 mmol/g. For the SiO 2 -supported K 2 CO 3 adsorbent pellets, the high calcination temperature (>700 °C) required to remove the graphite layer covering the pellet surface will cause the formation of new eutectics (i.e., K 2 Si 2 O 5 and K 2 Si 4 O 9 ), which leads to the collapse of the adsorbent pellets. Low calcination temperature of 500 °C can avoid the collapse of the SiO 2 -supported K 2 CO 3 adsorbent pellets and remove most of the graphite on the surface. Moreover, the CO 2 adsorption capacity can be further increased to 1.30 mmol/g by adding 20 wt% of microcrystalline cellulose to the SiO 2 -supported K 2 CO 3 adsorbent pellet. Although the adsorption capacity of structurally improved, SiO 2 -supported K 2 CO 3 pellets is still inferior to that of structurally improved, ZrO 2 -supported K 2 CO 3 pellets, they exhibit great cost advantage. Therefore, SiO 2 -supported K 2 CO 3 pellets with 20 wt% of microcrystalline cellulose have industrial application prospects.
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Polymers
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2022
·Vol. 14
·期 23
·5080
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IF 4.967
Leixuan Li,Yan Xin,Fengze Wu,Xiangrong Lyu,Qiyuan Yao,Xiaoting Yin,Qiang Zhang,Wenjuan Shan,Yong Chen,Qiuxia Han
CyclicN-halamines are highly antimicrobial, very stable, and not susceptible to bacterial resistance. A polysiloxane delivery vehicle was synthesized to deliver cyclic imideN-halamine onto cellulose via a benign and universal procedure that does not require a harmful solvent or chemical bonding. In brief, Knoevenagel condensation between barbituric acid and 4-hydroxybenzaldehyde furnished 5-(4-hydroxybenzylidene)pyrimidine-2,4,6-trione, whose phenolic O−H was subsequently reacted with the Si−H of poly(methylhydrosiloxane) (PMHS) via silane alcoholysis. The product of silane alcoholysis was interpenetrated into cellulose in supercritical CO2(scCO2) at 50 °C, to form a continuous modification layer. The thickness of the modification layer positively correlated with interpenetration pressure in the experimental range of 10 to 28 MPa and reached a maximum value of 76.5 nm, which demonstrates the ability for tunable delivery, to control the loading of the imide N−H bond originating from barbituric acid unit. The imide N−H bonds on cellulose with the thickest modifier were then chlorinated into N−Cl counterparts usingtert-butyl hypochlorite, to exert a powerful biocidability, providing ~7 log reductions of bothS. aureusandE. coliin 20 min. The stability and rechargeability of the biocidability were both very promising, suggesting that the polysiloxane modifier has a satisfactory chemical structure and interlocks firmly with cellulose via scCO2interpenetration.Keywords:cyclic imideN-halamines;polysiloxane;delivery vehicle;antibacterial surface;cellulose;scCO2interpenetration
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PubMed
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
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2022
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IF 3.656
Wen-Feng Zhou,Yi-Min Wei,Zhi-Wei Xiao,Yan Jiang,Yan-Kai Zhang,Zhen-Wei Zhang,Hui Hu,Longlong Geng,Da-Shuai Zhang,Yong-Zheng Zhang,Xiuling Zhang,Shujuan Zhuang
A new dual-cage-based porous metal-organic framework (MOF, termed DZU-113) assembly from the triazole-carboxylate linker and the Cu(II) paddle-wheel unit was solvothermally constructed. The structure of DZU-113 was determined by single-crystal X-ray diffraction, being consisted of the octahedral cage with an internal diameter of approximately 0.4 nm, and the spindle nano-cage with internal pores of about 0.8 nm × 2.2 nm, respectively. Specially, the uncoordinated N atoms of triazole groups are distributed in the bottleneck windows of the spindle nano-cage, serving as open functional sites. DZU-113 has permanent porosity with the Brunauer−Emmett−Teller surface area of 1207 m 2 g −1 . The CO 2 adsorption test demonstrated that the total uptake of DZU-113 can reach 66.7 cm 3 g −1 at 298 K, and 112.0 cm 3 g −1 at 273 K, 1 bar. Moreover, it achieves robust catalytic performance for the cycloaddition of CO 2 and epoxides under mild conditions.
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JOURNAL OF MOLECULAR LIQUIDS
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2023
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IF 6
Qiang Li,Fuling Wang,Yanling Wang,Baojun Bai,Jinyan Zhang,Cao Lili,Quan Sun,Yong Wang,Kobina Forson
Reducing the adsorption of CO 2 thickeners in soil particles of shallow shale is a pathway to protect the shale environment and water cycle. In this work, we first synthesized a siloxane-based thickener named AOB based on ring-opening polymerization and hydrosilylation reaction and discussed the influence of geological factors (including contents, pressure, temperature and shear rate) on the adsorption capacity of this thickener. The soil surface adsorption behavior of AOB was characterized by a self-assembled high-pressure soil adsorption device and the adsorption capacity was analyzed by Attenuated Total Reflectance Infrared Spectroscopy (ATR-FTIR). The results showed that AOB molecule belongs to the monolayer adsorption type on the soil surface by measuring the contents. Moreover, an inverse relationship was showed between pressure and adsorption capacity for AOB, while the significantly proportional relationship was presented for temperature and shear rate, respectively. It is found that the combined force formed by soil repulsion (originated from aromatic groups in AOB) and grid drag weakens the adsorption of AOB on the soil surface, resulting in a much lower adsorption capacity than the commercial PDMS. This work not only paves a new avenue for synthesizing siloxane-based polymer as CO 2 thickener, but also provides an efficient measure to reduce the adsorption of thickener on the shallow soil.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Yijie Wang,Hougang Fan,Xiaoyan Liu,Jian Cao,Huilian Liu,Xin Li,Lili Yang,Maobin Wei
Efficient electron transfer process and excellent CO 2 adsorption capacity are of great significance for improving CO 2 photoreduction efficiency. 3 D– 0 D ZnO/CsPbBr 3 S-scheme heterojunction hollow spheres were successfully prepared via a simple self-assembled process for efficient CO 2 photoreduction. Photocatalytic CO 2 reduction experiments showed that the ZnO/CsPbBr 3 had the excellent CO 2 photocatalytic conversion activity to CO, which was about 2.61 times higher than that of ZnO hollow micro-spheres and 1.9 times higher than that of pure CsPbBr 3 quantum dots (QDs). Photoelectrochemical characterization confirmed that the ZnO/CsPbBr 3 composite had good photoelectric conversion ability and carrier transfer ability, which was beneficial to the photocatalytic reaction. The suitable band gap structure and DFT calculation results showed that the formation of built-in electric field at the ZnO/CsPbBr 3 interface can greatly improve the S-scheme electron transfer ability, which can foster the CO 2 photoreduction. Besides, the introduction of 3D structure can improve the dispersion of CsPbBr 3 QDs and effectively enhance the CO 2 capture ability of the catalyst, which greatly promoted the CO 2 photoreduction reaction. The current work can present a novel S-scheme photocatalyst , which is looked forward to providing a certain perception into the advance of novel highly efficient CsPbBr 3 QDs-based photocatalysts for CO 2 resource utilization.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Changqing Guo,Guanghui Chen,Ning Wang,Shougui Wang,Yuwen Gao,Jipeng Dong,Qing Lu,Fei Gao
Several novel multifunctional histidine-based hypercrosslinked ionic polymers (HIPs) were constructed via a one-pot copolymerization strategy. The resultant HIPs were characterized by various technologies and investigated for the CO 2 adsorption and conversion. Plentiful hydrogen bond donors, nucleophilic ionic sites, and Lewis bases were successfully integrated into the HIPs skeletons. As-prepared histidine-based HIPs possess excellent hierarchical pore structure. The optimal HIP-Br-His exhibits a high CO 2 capture capacity of 2.90 mmol/g at 273 K and 1 bar, much higher than that of corresponding hypercrosslinked polymer HCP-Br without histidine units. Meanwhile, the HIP-Br-His achieves an excellent catalytic activity of 95 % product yield with 99 % product selectivity in CO 2 cycloaddition to propylene oxide under metal-, cocatalyst- and solvent-free and mild conditions (70 °C and 1.0 MPa). Particularly, HIP-Br-His can efficiently capture and convert dilute CO 2 into cyclic carbonates with a satisfactory catalytic performance. The excellent catalytic activity associating with the confirmed good stability, recyclability, and substrate compatibility make the developed histidine-based HIPs a promising heterogeneous catalyst for efficient CO 2 capture and conversion.
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ENERGY
·
2023
·
IF 9
Xinwei He,Hang He,Francesco Barzagli,Mohammad Waleed Amer,Chao'en Li,Rui Zhang
Blending two or more amines has recently been recognized as an efficient strategy to formulate competitive sorbents for post-combustion CO 2 capture, as it allows to benefit from the advantages of each individual amine. In the present work, we devised four new dual-amine aqueous blends, based on the tertiary amine 2-dimethylamino-2-methyl-1-propanol (2DMA2M1P) mixed with different primary and secondary amines , namely ethanolamine (MEA), benzylamine (BZA), 2-amino-2-methyl-1-propanol (AMP) and diethanolamine (DEA). The CO 2 capture and release performance of the formulated blends were experimentally evaluated by measuring CO 2 equilibrium solubility, CO 2 absorption and desorption rates, and energy consumption during the regeneration process, and results were compared with those obtained under the same operating conditions with 5 M aqueous MEA, the reference sorbent for CO 2 capture processes. Moreover, 13 C NMR spectroscopy was used to identify and quantify the species formed during the CO 2 absorption process to better understand the reaction mechanism in each blend. We found that all formulated blends showed appreciable CO 2 capture performance and, most importantly, significantly better desorption performance than conventional MEA. In particular, BZA+2DMA2M1P provided the best capture performance, while AMP+2DMA2M1P showed a faster CO 2 desorption rate and lower energy consumption than the other tested blends.
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ACS Applied Materials & Interfaces
·
2023
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IF 9.5
Chan Yang,Yarong Hu,Sanxiu Li,Qun Huang,Juan Peng
Electrocatalytic reduction of CO2 into valuable fuels and chemical feedstocks in a sustainable and environmentally friendly manner is an ideal way to mitigate climate change and environmental problems. Here, we fabricated a series of self-supporting Bi–Sb bimetallic nanoleaves on carbon paper (CP) by a facile electrodeposition method. The synergistic effect of Bi and Sb components and the change of the electronic structure lead to high formate selectivity and excellent stability in the electrochemical CO2 reduction reaction (CO2RR). Specifically, the Bi–Sb/CP bimetallic electrode achieved a high Faradic efficiency (FEformate, 88.30%) at −0.9 V (vs RHE). The FE of formate remained above 80% in a broad potential range of −0.9 to −1.3 V (vs RHE), while FECO was suppressed below 6%. Density functional theory calculations showed that Bi(012)–Sb reduced the adsorption energy of the *OCHO intermediate and promoted the mass transfer of charges. The optimally adsorbed *OCHO intermediate promoted formate production while inhibiting the CO product pathway, thereby enhancing the selectivity to formate synthesis. Moreover, the CO2RR performance was also investigated in a flow-cell system to evaluate its potential for industrial applications. The bimetallic Bi–Sb catalyst can maintain a steady current density of 160 mA/cm2 at −1.2 V (vs RHE) for 25 h continuous electrolysis. Such excellent stability for formate generation in flow cells has rarely been reported in previous studies. This work offers new insights into the development of bimetallic self-supporting electrodes for CO2 reduction.
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