ACS Omega
·
2024
·
IF 3.7
Kai Shan,Zhengsong Qiu,Qi Yin,Qingzhen Cui,Dandan Su,Hanyi Zhong,Xin Zhao
For the purpose of efficient temporary plugging and self-removal of the plugging of reservoir formations, the thermally induced expandable and acid-generating temporary plugging agent (TAPA) was prepared with acrylonitrile (AN), methacrylic acid (MAA), N,N-dimethylacrylamide (DMAA), and butyl acrylate (BA) as the shell monomers as well as the carboxylate esters with high boiling points as the core material. The TAPA was structurally characterized, and the properties were studied. The results showed that the TAPA had a good spherical structure with a median particle size (D50) of 16.03 μm. The initial expansion temperature Tstart of the TAPA was 134.75 °C, and its maximum expansion temperature Tmax was 197.77 °C. The surface was hydrophilic and negatively charged, with excellent shear strength and sealing. The TAPA was suitable for temporary plugging and self-removal of the plugging of the reservoir formation with a temperature of 160 °C. The release of core materials and the effect on self-removal of plugging were not significantly affected with different salinities, weak acid or weak alkali environments, or a small quantity of hydrocarbons. With addition of 1–3 wt % TAPA, the rheological property of water-based drilling fluid changed slightly, but the filtration loss reduced, suggesting a good compatibility of the TAPA with the drilling fluid. Results of plugging and plugging removal experiments in fractured reservoir formations and permeable reservoir formations showed that the TAPA improved the strength of the temporary plugging layer with the elastic deformation due to thermal expansion and realized self-removal of the plugging by corroding the temporary plugging layer with carboxylic acid hydrolyzed from the carboxylic ester released, thereby decreasing the backflow pressure of oil and gas wells in the production stage. The results provided a new method and technological idea for efficient temporary plugging and self-removal of the plugging of reservoir formations.
研究领域:
石油工程
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材料科学
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产品关联
DOI
PubMed
高影响因子
Reaction Chemistry & Engineering
·
2025
·
IF 3.1
Rihong Liu,Baicheng Feng,Fanuan Yu,Huifen Xin,Rong Qu,Yan Jin
This paper presents the design and synthesis of nine ionic photogenerating acid generators (PAGs) based on iodonium salts. The compounds were characterized using 1H NMR, 13C NMR, 19F NMR and UV, the structures and properties of 9 PAGs molecules were determined. The maximum ultraviolet absorption wavelength of each PAGs is in the range of 200-250nm, with a wide absorption domain, making it highly applicable. In addition, Using the uneven discoloration of Rhodamine B (RB) in the presence of acid, the acid production efficiency of 9 PAGs under 254nm ultraviolet irradiation was quantitatively measured in acetonitrile. It was found that all 9 PAGs underwent I-C cleavage and generated specific acids and other photolysis products. The mechanism for the heteroclitic cleavage of the I-C bond to generate acid was backed by calculations using time-dependent density functional theory (TD-DFT).
研究领域:
化学
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材料科学
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光化学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Liu Yang,Shang Huishan,Zhang Bing,Yan Dongpeng,Xiang Xu
The C–C bond cleavage of biomass-derived glycerol to generate value-added C1 products remains challenging owing to its slow kinetics. We propose a surface fluorination strategy to construct dynamic dual hydrogen bonds on a semiconducting BiVO 4 photoelectrode to overcome the kinetic limit of the oxidation of glycerol to produce formic acid (FA) in acidic media. Intensive spectroscopic characterizations confirm that double hydrogen bonds are formed by the interaction of the F–Bi–F sites of modified BiVO 4 with water molecules, and the unique structure promotes the generation of hydroxyl radicals under light irradiation, which accelerates the kinetics of C–C bond cleavage. Theoretical investigations and infrared adsorption spectroscopy reveal that the double hydrogen bond enhances the C=O adsorption of the key intermediate product 1,3-dihydroxyacetone on the Bi–O sites to initiate the FA pathway. We fabricated a self-powered tandem device with an FA selectivity of 79% at the anode and a solar-to-H 2 conversion efficiency of 5.8% at the cathode, and these results are superior to most reported results in acidic electrolytes.
研究领域:
材料科学
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光电化学
·
催化反应
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF POROUS MATERIALS
·
2017
·Vol. 25
·期 4
·1027-1034
·
IF 1.624
Chen Yongquan,Yang Haitao,Nie Jun,Zhu Xiaoqun
Highly flexible silica aerogels were fabricated by using 2-(3-(triethoxysilyl)propylcarbamoyloxy) ethyl acrylate (TESEA), methyltriethoxysilane (MTES), and polydimethylsiloxane (PDMS) as co-precursors through photopolymerization and sol–gel process, then followed by ambient pressure drying. Attributing to photolysis of the photoacids generators, the radical and Brönsted acid (HSbF 6 ) were generated simultaneously under irradiation. The radical initiated the photopolymerization of acrylate which induced the gelation and fixed the shape of the gel quickly, the acid allowed the sol–gel process occurring gradually. Due to the enhancement of the polymer, the strength of aerogels was improved. The aerogels had low density (~ 0.098 g/cm 3 ), high porosity (~ 94.8%), high flexibility and high elastic recovery. Moreover, the silica aerogels have hydrophobic and oleophilic properties, which endows them with an ability of oil water separation.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2019
·Vol. 24
·期 11
·2119
·
IF 3.06
Lijun Zhang,Berlin Zang,Chundong Huang,Jun Ren,Lingyun Jia
Dialysis-related amyloidosis (DRA), which has been widely recognized to be associated with the accumulation of β2-microglobulin (β2-m) in blood, is one of the most common complications in patients receiving long-term dialysis treatment. The most significant side-effect of existing hemodialysis sorbents for the removal of β2-m from blood is the loss of vital proteins due to non-specific adsorptions. Although the traditional antibodies have the capability to specifically remove β2-m from blood, high cost limits their applications in clinics. Single domain antibodies derived from the Camelidae species serve as a superior choice in the preparation of immunoadsorbents due to their small size, high stability, amenability, simplicity of expression in microbes, and high affinity to recognize and interact with β2-m. In this study, we modified the anti-β2-m VHH by the formylglycine-generating enzyme (FGE), and then directly immobilized the aldehyde-modified VHH to the amino-activated beads. Notably, the fabrication is cost- and time-effective, since all the preparation steps were performed in the crude cell extract without rigorous purification. The accordingly prepared immunoadsorbent with VHHs as ligands exhibited the high capacity of β2-m (0.75 mg/mL). In conclusion, the VHH antibodies were successfully used as affinity ligands in the preparation of novel immunoadsorbents by the site-specific immobilization, and effectively adsorbed β2-m from blood, therefore opening a new avenue for efficient hemodialysis.Keywords:β2-microglobulin;VHH;formylglycine-generating enzyme;hemodialysis
研究领域:
生物医学工程
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分子生物学
·
透析治疗
✓ 已验证
DOI
PubMed
高影响因子
FUEL
·
2022
·
IF 8.035
Baicheng Feng,Zichen Zhang,Jiaqiang Wang,Donglin Yang,Qun Li,Yaping Liu,Hengjun Gai,Tingting Huang,Hongbing Song
The catalytic hydrogenation of carbon dioxide (CO 2 ) into formic acid is among the most important reactions to alleviate global warming and realize the carbon cycle. How to achieve rapid activation of CO 2 remains a challenge. In this work, we designed two novel hydrophobic poly(ionic liquid)s (PILs) with a good affinity for CO 2 . Since the abundant N atoms in the PILs can anchor palladium (Pd) nanoparticles, the designed catalyst can rapidly activate CO 2 and H 2 simultaneously, thus efficiently catalyzing the hydrogenation of CO 2 to formic acid under mild conditions. Due to the synergy from the bis(trifluoromethanesulfonyl)amide anion ([Tf 2 N − ]) with strong hydrophobicity and CO 2 affinity and trimethylamine (NEt 3 ) as a low dissociation energy alkaline additive, the resultant Pd/PIL-bip-Tf 2 N exhibited the best catalytic performance on the hydrogenation of CO 2 to formic acid. The TOF value reached 1,190 h −1 in the aqueous solution of NEt 3 at 100 °C, 1 h, and a total pressure of 4 MPa. The activation energy and dissociation energy during the catalytic process were calculated by DFT, indicating that the synergistic effect of NEt 3 is better than that of other alkaline additives. In addition, the catalytic activity of the catalyst remained stable after several cycling experiments. Based on the obtained results, we proposed a possible reaction pathway. Therefore, PILs have great potential as catalyst carrier material for CO 2 hydrogenation.
研究领域:
化学
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材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Frontiers in Bioengineering and Biotechnology
·
2019
·
IF 5.122
Li Yan,Wen Liyin,Tan Tianwei,Lv Yongqin
The main challenges in multienzymatic cascade reactions for CO2 reduction are the low CO2 solubility in water, the adjustment of substrate channeling, and the regeneration of co-factor. In this study, metal-organic frameworks (MOFs) were prepared as adsorbents for the storage of CO2 and at the same time as solid supports for the sequential co-immobilization of multienzymes via a layer-by-layer self-assembly approach. Amine-functionalized MIL-101(Cr) was synthesized for the adsorption of CO2. Using amine-MIL-101(Cr) as the core, two HKUST-1 layers were then fabricated for the immobilization of three enzymes chosen for the reduction of CO2 to formate. Carbonic anhydrase was encapsulated in the inner HKUST-1 layer and hydrated the released CO2 to HCO3-. Bicarbonate ions then migrated directly to the outer HKUST-1 shell containing formate dehydrogenase and were converted to formate. Glutamate dehydrogenase on the outer MOF layer achieved the regeneration of co-factor. Compared with free enzymes in solution using the bubbled CO2 as substrate, the immobilized enzymes using stored CO2 as substrate exhibited 13.1-times higher of formate production due to the enhanced substrate concentration. The sequential immobilization of enzymes also facilitated the channeling of substrate and eventually enabled higher catalytic efficiency with a co-factor-based formate yield of 179.8%. The immobilized enzymes showed good operational stability and reusability with a cofactor cumulative formate yield of 1077.7% after 10 cycles of reusing.
研究领域:
生物化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Yinuo Wang,Hongming Xu,Ernest P. Delmo,Juhee Jang,Yan Zhang,Tiehuai Li,Xiaoyi Qiu,Zhehan Ying,Ping Gao,Minhua Shao
Electrochemical reduction of CO2 to formic acid for industrial production necessitates not only high selectivity and conversion rate but also efficient CO2 utilization and minimal carbon loss to reduce overall production costs and energy consumption. Despite acidic CO2 reduction reaction being able to greatly alleviate carbon loss, it is often hindered by the aggressive hydrogen evolution reaction and the degradation of catalysts. This study puts forward an effective fluorination-hydrolysis protection mechanism for Sn-based electrocatalysts under acidic conditions. F-doped Sn oxides form a protective layer containing Sn oxide and fluoride, which safeguards the inner reduced Sn from significant degradation in acidic environments. Leveraging this strategy, we achieve impressive performance for formic acid generation without the adverse effects of a violent hydrogen evolution reaction during acidic electrolysis, attaining a Faradaic efficiency of 92% and a partial current density of 722 mA cm–2. This approach not only provides an additional avenue for preventing corrosion of Sn-based catalysts in acidic media but also significantly improves their performance in formic acid production.
研究领域:
电化学
·
材料科学
·
能源转化
✓ 已验证
产品关联
DOI
高影响因子
Nano Energy
·
2019
·
IF 15.548
Yecan Pi,Jun Guo,Qi Shao,Xiaoqing Huang
Perovskite oxides are a class of attractive materials for their broad applications in many energy conversion and storage fields, while their catalytic performance of CO 2 electroreduction (CO 2 ER) has been rarely investigated. Herein, all-inorganic SrSnO 3 perovskite nanowires are constructed and utilized to catalyze the CO 2 ER for the first time. Inspiringly, such SrSnO 3 NWs demonstrates impressive selectivity and activity for formate production, with considerable Faradaic efficiencies (~80%) over a broad potential range, and the highest formate partial current density of 21.6 mA cm −2 , much better than that of the SnO 2 nanoparticles . Further analyses reveal that the notable CO 2 ER activity of SrSnO 3 NWs is linked to the efficient stabilization of formate intermediate (CO 2 •− ) as well as the slow kinetics for hydrogen evolution reaction (HER). This work can inspire the development of highly efficient perovskite catalysts for CO 2 ER and beyond.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Xuetong Liu,Chi Zhang,Nuoyan Li,Runfeng Li,Songlin Lei,Wei Hong,Shuguang Deng,Jun Wang
Herein, a novel and flexible self-supporting gas diffusion electrode (GDE) was fabricated, which including an electrodeposited Bi nanocomposite as a catalyst layer and MIL-101 derived porous carbon in the gas diffusion layer (GDL). Compared with the conventional fabrication of GDE electrodes, the electrodeposition approach can avoid the tedious drop-casting processes of the catalyst layer (CL). The in situ growth mode by electrodeposition can also ensure the firmly interaction between CL and current collector, thus enhancing the stability of the electrode. Meanwhile, the porous carbon derived from MIL-101 which with a high specific area is conducive for the CO 2 enrichment on the electrode, thus facilitate the reaction with high current density. Owe to the special structure, the resultant catalyst showed excellent performance for electrocatalytic CO 2 reduction reaction (CO 2 RR) with enhanced formic acid generation. Notably, at -1.37 V ( vs. RHE), a large current density of 400 mA cm -2 and a high formate Faraday efficiency (FE formate ) of 96.5 % were achieved, and the yield of formic acid reached 46.5 mmol cm -2 h -1 , which is superior to most electrocatalytic catalysts for CO 2 RR. In addition, the FE formate value remained high (>90 %) over a wide voltage window of 800 mV, and the catalyst also maintained stable operation at industrial current density for 70 h. This work provides a new strategy for the design of GDEs with novel structure to achieve high activity and durability for different electrocatalysis.
研究领域:
电化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Frontiers in Microbiology
·
2018
·
IF 4.019
Mi Lan,Yang Bin,Hu Xialu,Luo Yang,Liu Jianxin,Yu Zhongtang,Wang Jiakun
The rumen and the hindgut represent two different fermentation organs in herbivorous mammals, with the former producing much more methane than the latter. The objective of this study was to elucidate the microbial underpinning of such differential methane outputs between these two digestive organs. Methane production was measured from 5 adult sheep and 15 adult rabbits, both of which were placed in open-circuit respiratory chambers and fed the same diet (alfalfa hay). The sheep produced more methane than the rabbits per unit of metabolic body weight, digestible neutral detergent fiber, and acid detergent fiber. pH in the sheep rumen was more than 1 unit higher than that in the rabbit cecum. The acetate to propionate ratio in the rabbit cecum was more than threefold greater than that in the sheep rumen. Comparative analysis of 16S rRNA gene amplicon libraries revealed distinct microbiota between the rumen of sheep and the cecum of rabbits. Hydrogen-producing fibrolytic bacteria, especially Butyrivibrio, Succiniclastium, Mogibacterium, Prevotella, and Christensenellaceae, were more predominant in the sheep rumen, whereas non-hydrogen producing fibrolytic bacteria, such as Bacteroides, were more predominant in the rabbit cecum. The rabbit cecum had a greater predominance of acetogens, such as those in the genus Blautia, order Clostridiales, and family Ruminococcaceae. The differences in the occurrence of hydrogen-metabolizing bacteria probably explain much of the differential methane outputs from the rumen and the cecum. Future research using metatranscriptomics and metabolomics shall help confirm this premise and understand the factors that shape the differential microbiota between the two digestive organs. Furthermore, our present study strongly suggests the presence of new fibrolytic bacteria in the rabbit cecum, which may explain the stronger fibrolytic activities therein.
研究领域:
微生物学
·
动物科学
·
环境科学
✓ 已验证
DOI
PubMed
高影响因子
Scientific Reports
·
2015
·Vol. 5
·期 1
·1-10
·
IF 5.578
Qiao Sen,Tian Tian,Qi Benyu,Zhou Jiti
This study presents a novel procedure for accelerating methanogenesis from wastewater by adding elemental manganese into the anaerobic digestion system. The results indicated that elemental manganese effectively enhanced both the methane yield and the production rate. Compared to the control test without elemental manganese, the total methane yield and production rate with 4 g/L manganese addition increased 3.4-fold (from 0.89 ± 0.03 to 2.99 ± 0.37 M/gVSS within 120 h) and 4.4-fold (from 6.2 ± 0.1 to 27.2 ± 2.2 mM/gVSS/h), respectively. Besides, more acetate consumption and less propionate generation were observed during the methanogenesis with manganese. Further studies demonstrated that the elemental manganese served as electron donors for the methanogenesis from carbon dioxide and the final proportion of methane in the total generated gas with 4 g/L manganese addition reached 96.9%, which was 2.1-fold than that of the control (46.6%).
研究领域:
环境工程
·
生物技术
·
微生物学
✓ 已验证
DOI
PubMed
高影响因子
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