COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Chunhua Liang,Chuantao Wang,Kaixuan Xu,Hongbin He,Qiangen Li,Chunming Yang,Xiaoming Gao
The benzaldehyde (BAD) produced by the benzyl alcohol (BA) oxidation method is comprehensively applied to food and pharmaceutical fields. However, the selectivity and conversion of photocatalytic selective oxidation of BA in aqueous solution are still far from expectation. Herein, N-CQDs/CdS composites were synthesized by the in-situ precipitation method. N-CQDs served as an "Electronic Warehouse" to boost the separation efficiency of the carrier. The electron transferred from CdS to N-CQDs made electron on the N-CQDs surface enrich, which was conducive to the formation of superoxide radicals (·O 2 - ).·O 2 - and h + could efficiently oxidize BA to BAD. In addition, according to density functional theory (DFT), the adsorption energies of BA and BAD on N-CQDs/CdS were distinctly greater than that of CdS. BAD tended to desorb from the 7.5 N-CQDs/CdS surface, and BA preferred to adsorb on the CdS surface. However, BAD was difficult to desorb from the CdS surface, resulting in the poisoning of CdS. 7.5 N-CQDs/CdS exhibited the BA conversion of 60.4% and BAD selectivity of 99%, which was 2.2 times higher than that of original CdS. This work was expected to provide a theoretical basis for improving photocatalyst carrier separation efficiency and alcohol selective oxidation performance.
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Fundamental Research
·
2022
·
IF 0
Feng Ma,Xuan Liu,Xiaoming Wang,Jiashun Liang,Jianyu Huang,Cameron Priest,Jinjia Liu,Shuhong Jiao,Tanyuan Wang,Gang Wu,Yunhui Huang,Qing Li
Transition metal supported N-doped carbon (M-N-C) catalysts for oxygen reduction reaction (ORR) are viewed as the promising candidate to replace Pt-group metal (PGM) for proton exchange membrane fuel cells (PEMFCs). However, the stability of M-N-C is extremely challenging due to the demetalation, H 2 O 2 attack, etc. in the strongly oxidative conditions of PEMFCs. In this study, we demonstrate the universal effect of Zn on promoting the stability of atomically dispersed M-N x /C (M = Co, Fe, Mn) catalysts and the enhancement mechanism is unveiled for the first time. The best-performing dual-metal-site Zn-Co-N-C catalyst exhibits a high half-wave potential ( E 1/2 ) value of 0.81 V vs. reversible hydrogen electrode (RHE) in acid and outstanding durability with no activity decay after 15,000 accelerated degradation test (ADT) cycles at 60 °C, surpassing most reported Co-based PGM-free catalysts in acid media. For comparison, the Co-N-C in the absence of Zn suffers from a rapid degradation after ADT due to the demetalation and higher H 2 O 2 yield. X-ray adsorption spectroscopy (XAS) and density functional theory (DFT) calculations suggest the more negative formation energy (by 1.2 eV) and increased charge transfer of Zn-Co dual-site structure compared to Co-N-C could strength the Co-N bonds against the demetalation and the optimized d-band center accounts for the improved ORR kinetics.
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MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 9
·1-10
·
IF 6.408
Wang Yuexin,Chen Rui,Shen Bo,Li Cai,Chen Junman,Wang Yanshuang,Tian Shen,Li Xuemiao,Luo Nini,Liu Rui,Ding Shijia,Zhu Chuanlong,Xia Qianfeng
A multifunctional catalytic nanomaterial (Co-MOF@AuNP@ABEI) composed of cobalt-doped metal–organic frameworks (Co-MOF), gold nanoparticles (AuNP), and N -(4-aminobutyl)- N -(ethylisoluminol) (ABEI) is reported. Co-MOF@AuNP@ABEI exhibits high synergistic and zero-distance catalytic properties, which are beneficial to the improvement of the detection sensitivity of an electrochemiluminescent (ECL) biosensor. After coupling with the ECL system and 3D magnetic walking nanomachine amplification strategy, the Co-MOF@AuNP@ABEI can achieve an ultrasensitive ECL assay of Burkholderia pseudomallei with the limit of detection (LOD) of 60.3 aM, which is 2 and 4 orders of magnitude lower than individual ECL system without the nanomachine (4.97 fM) and individual walking nanomachine (340 fM), and superior to the pathogenic bacteria analyses in the previous report. Moreover, the LOD of the proposed ECL detection system for the determination of B. pseudomallei in serum sample was as low as 9.0 CFU mL −1 . The relative standard deviations (RSD) of ECL intensity for the detection of five B. pseudomallei -spiked serum samples were 4.02%, 0.84%, 0.84%, 1.55%, and 0.21%, respectively. The recoveries of the ECL biosensor for the detection of B. pseudomallei DNA-spiked serum samples were 93.63 ~ 107.83%. Therefore, this work demonstrated that the developed multifunctional catalytic nanomaterial with synergistic and zero-distance catalytic properties can be used as excellent ECL signal reporter to improve the detection sensitivity of ECL biosensor. Graphical abstract
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Siming Ren,Mingjun Cui,Xinyu Chen,Shixiang Mei,Yujie Qiang
Carbon steel is the most widely used engineering material , and its corrosion is one of the main areas of concern in many industries. The most practical approach to control this problem is to use corrosion inhibitors . Currently, because of their good water solubility, excellent chemical stability, low cost and nontoxic features, carbon dots (CDs), especially heteroatom-doped CDs, have been developed as green corrosion inhibitors, but the corrosion inhibition efficiency and underlying mechanisms of single- or dual-element doping have not yet been accurately compared and analyzed. Inspired by this, eco-friendly nitrogen-doped and nitrogen, sulfur codoped CDs ( N -CDs and N,S-CDs) are prepared via a one-step hydrothermal process, and a comparative study on their inhibition performance for carbon steel corrosion in strong acidic solution is performed. The results show that both N -CDs and N,S-CDs can restrain the corrosion of carbon steel, and their inhibition efficiency increases with increasing concentration and immersion time, reaching approximately 87.9% ( N -CDs) and 96.4% (N,S-CDs) at 200 ppm after 1 h of immersion. Molecular dynamics simulation indicates that the strong interaction ability between N,S-CDs and the Fe substrate leads to higher corrosion inhibition performance than the single N doping case, benefiting from the multi-anchor adsorption of N,S-CDs on carbon steel in a strong acidic solution. Therefore, the facile preparation, eco-friendliness and high corrosion inhibition performance of N,S-CDs will provide a new approach for designing highly efficient carbon dots and broadening the application of carbon dots in the corrosion field.
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PubMed
高影响因子
Carbon Energy
·
2022
·Vol. 5
·期 2
·e257
·
IF 21.556
Yihua Tang,Jingjing Chen,Zhiyong Mao,Christina Roth,Dajian Wang
N-doped carbons as one of the most prominent anode materials to replace standard graphite exhibit outstanding Li + storage performance. However, N-doped carbon anodes still suffer from low N-doping levels and low initial Coulombic efficiency (ICE). In this study, high N-doped and low graphitic-N carbons (LGNCs) with enhanced ICE were synthesized by taking advantage of a denitrification strategy for graphitic carbon nitride (g-C 3 N 4 ). In brief, more than 14.5 at% of N from g-C 3 N 4 (55.1 at% N) was retained by reacting graphitic-N with lithium, which was subsequently removed. As graphitic-N is largely responsible for the irreversible capacity, the anode's performance was significantly increased. Compared to general N-doped carbons with high graphitic-N proportion (>50%) and low N content (<15 at%), LGNCs delivered a low proportion of 10.8%–17.2% within the high N-doping content of 14.5–42.7 at%, leading to an enhanced specific capacity of 1499.9 mAh g −1 at an ICE of 93.7% for the optimal sample of LGNC (4:1). This study provides a facile strategy to control the N content and speciation, achieving both high Li + storage capacity and high ICE, and thus promoting research and application of N-doped carbon materials.
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高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2021
·
IF 2.694
Bingjie Huo,Xiaomin Qiu,Hongru Zhang,Yaning Zhang,Jingwei Yang,Zhaoyou Zhu,Yinglong Wang,Jun Gao
Isoamyl butyrate is a common food additive. Water will be generated by esterification reaction in the process of its formation. Cyclohexane, n-hexane, and n-heptane are often selected as entrainers to remove water and promote the reaction. In this work, the vapor–liquid equilibrium data of the binary systems of isoamyl alcohol + isoamyl butyrate, cyclohexane + isoamyl butyrate, n-hexane + isoamyl butyrate, and n-heptane + isoamyl butyrate were determined by using a modified Rose vapor recirculating-type equilibrium still at 101.3 kPa. Fredenslund test and Van Ness point test methods are used to verify the thermodynamic consistency of the experimental vapor–liquid equilibrium data. In addition, three classical activity coefficient models, Wilson, NRTL, and UNIQUAC, were used to fit the isobaric vapor–liquid equilibrium data of four binary systems. The binary interaction parameters were obtained by regression of experimental data.
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高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2021
·Vol. 138
·期 39
·51001
·
IF 3.125
Guoshuai Wang,Guancheng Jiang,Jun Yang,Lili Yang,Xinliang Li,Yinbo He,Xiangyang Chang
Ultra-high temperature dramatically deteriorates rheological properties and filtration performance of water-based drilling fluids (WBDFs), especially for a salt-gypsum formation that greatly restricts the application of WBDFs in ultra-deep well drilling operations. Hence, the research in this article used an anionic copolymer (DANS) prepared by N , N -dimethylacrylamide, 2-acrylamide-2-methylpropanesulfonic acid, N -vinylpyrrolidone, and sodium 4-styrenesulfonate as an anti-ultra-high temperature and anti-salt contamination filtrate reducer. Due to its multiple bulky cyclic structures in the side chain, DANS exhibits excellent thermal stability in the thermal gravimetric, rheological, and filtration tests. By adding 1.0 wt% DANS, the American Petroleum Institute (API) filtration volume of sodium bentonite-based fluids (SBT-BFs) decreased from 56.0 to 9.2 ml after aging at 240°C. Even under both 20 wt% NaCl contamination and 240°C aging, SBT-BFs with 2.0 wt% DANS could maintain a filtration volume of 9.4 ml, whereas SBT-BFs without DANS reached a filtration volume of 203.0 ml. The possible filtration control mechanism of DANS was further investigated via the Fourier transform infrared spectroscopy (FTIR), atomic force microscopy (AFM), ζ potential, particle size distribution, filter cake micro-morphology, and transmission electron microscopy (TEM). Confirmed by FTIR and AFM results, the effective adsorption was formed between DANS and bentonite even under a high-salinity environment. Thus, a firm “dot net” structure formed by bentonite/DANS was observed by TEM, significantly improving the colloidal stability, dispersibility, and filter cake compactness of SBT-BFs. Finally, by utilizing DANS as the core treatment agent, a high-density WBDFs system with a temperature resistance of 240°C and a salt-tolerance of 20 wt% has been successfully prepared.
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Molecular Catalysis
·
2021
·
IF 5.062
Yanyan Guo,Yichun Dong,Zhigang Lei,Zhixue Liu,Jiqin Zhu
The catalytic performance of Pd-N/Silicon Dioxide/Cordierite (Pd-N/SD/C) ( N = Ga and Ag) bimetallic monolithic catalysts for 2-ethylanthraquinone (eAQ) hydrogenation was investigated. Catalyst characterization by HRTEM, XPS, and TPR reveal that Pd-Ga/SD/C can form an alloy structure to produce significant synergetic effects. Moreover, the use of different Pd/Ga mass ratio in catalysts reveals that when the mass ratio of Pd and Ga/Ag = 2:1, Pd-Ga/SD/C obtains the highest yield of H 2 O 2 and selectivity toward active quinones, which can reach 7.4 g L −1 and 90%. Moreover, to have a deep understanding of the eAQ-PdN(1 1 1) or eAQ-Pd(1 1 1) interaction mechanism, the calculation of eAQ adsorption on Pd-N/SD/C catalysts surface was performed by density functional theory (DFT). It is shown that the higher catalytic activity over Pd-Ga/SD/C is due to the stronger carbonyl group of eAQ adsorption on Pd 3 Ga 1 (1 1 1).
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2021
·
IF 5.316
Wei Liu,Liang-Min Ning,Shao-Qing Li,Wei-Xing Liu,Qiang Zhang,Jia Shao,Jin-Lei Tian
A rational and convenient strategy was designed to synthesize high level N-doped Co@NCNTs composites derived from adenine-based AD-MOF-1 and Bio-MOF-11 via one-step pyrolysis method. Adenine can be used as an endogenous nitrogen source to apparently increase the N content of the materials. N-rich CNTs form a protecting layer for Co nanoparticles to avoid the aggregation of metal nanoparticles . The abundant nitrogen content can enhance electronic conductivity and bring additional active sites. The prepared Co@NCNTs display high catalytic efficiency for various nitro aromatics reduction in aqueous solution. The Co@NCNT-1-800 implies outstanding catalytic efficiency of 96% for the reduction of 4-NP. A mechanistic analysis revealed the abundant Co catalytic sites on the surface of catalysts to promote electron transfer efficiency and improve catalytic performance significantly. Moreover, the magnetic Co-based catalysts remained excellent catalytic activity and reusability even after five cycles.
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高影响因子
BIOCHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 3.475
Changsen Li,Xianxiu Li,Yang Liu,Yan Sun
Our previous study reported a novel protein ion-exchanger, N,N-dimethylaminopropyl acrylamide (DMAPAA)-grafted Sepharose FF, of very high protein adsorption capacity and uptake rate. To gain new insight into the polymer grafting effects on protein adsorption and chromatography, 18 DMAPAA-grafted anion exchangers of four grafting densities and various chain lengths (i.e., ionic capacities, ICs) were prepared and named as FF-Br x -pDMAPAA n ( x represents grafting density and n stands for IC in mmol/L). It was found that an optimal IC existed at each grafting density to present a maximal capacity. Of the four optimal-IC resins, FF-Br3-pDMAPAA587 showed the highest capacity (377 mg/mL), but the protein uptake rate, defined as the ratio of effective pore diffusivity to free diffusivity ( D e / D 0 ), was smaller than the resin of a similar ionic capacity but lower grafting density (FF-Br2-pDMAPAA592). Consequently, the dynamic binding capacity (DBC) of FF-Br2-pDMAPAA592 was higher than that of FF-Br3-pDMAPAA587 at flow velocities higher than 450 cm/h. Moreover, FF-Br3-pDMAPAA587 showed higher adsorption capacity than FF-Br2-pDMAPAA592 at 0−150 mmol/L NaCl, leading to its higher DBC values as compared to FF-Br2-pDMAPAA592 in the same salt concentration range. Taken together, DMAPAA-grafted resins of different grafting densities would be useful for purifying feedstocks of different ionic strengths.
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高影响因子
OPTIK
·
2020
·
IF 2.187
Tongpeng Zhao,Shaohua Ji,Degao Zhong,Fei Teng,Shakir Ullah,Siyuan Hu,Jie Tang,Bing Teng
The organic nonlinear optical (NLO) material N, N-dimethyl-4-[2-(2-quinolyl) vinyl] aniline (DADMQ) has been synthesized and high-quality single crystal with the dimension of 8 × 1 × 0.5 mm 3 was grown from methanol solvent by slow cooling method for the first time. Single crystal and powder XRD studies show that DADMQ crystal belongs to the orthorhombic space group Pna2 1 . All the functional groups and structure of the synthetic material can be determined from FT-IR and 1 H NMR spectral analyses. The thermal properties can be studied through TG/DTG and DSC analyses, and its melting point is confirmed at 184.9 ℃. Some critical optical characteristics like the optical transmittance, optical absorption coefficient (α), energy band gap ( E g ), cut-off wavelength (λ max ) and extinction coefficient (κ) can be carried out through UV–vis-NIR spectral analysis. The dielectric features of the title crystal have also been measured. Furthermore, there is a blue emission appeared at 493 nm through PL spectral analysis. The second harmonic generation (SHG) efficiency of the title crystal has been measured, which indicates that DADMQ has 3.64 times greater than KDP crystal.
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高影响因子
Journal of Rubber Research
·
2019
·Vol. 23
·期 1
·41-46
·
IF 0.281
Liao Xiao-Xue,Wei Yan-Chan,Zhang Hui-Feng,Zheng Ting-Ting,Luo Ming-Chao,Liao Shuangquan
Waste rubber with three-dimensional structure is insoluble and non-melting, which creates recycling problem. The technique called “high-pressure high-temperature sintering” (HPHTS) can convert vulcanized rubber powder into usable rubber products. However, reversion occurs when vulcanizates are exposed to a prolonged treatment at high temperature. This reversion results in the decrease of mechanical properties of sintered waste rubber powder (WRP) samples. To address this problem, a method of enhancing the mechanical properties of sintered WRP by incorporating different content of maleic anhydride (MA) and N , N ′- m -phenylene bismaleimide (BMI) is discussed in this paper. The results show that BMI and MA can slow down the formation of the conjugated double bonds. Through Diels–Alder reaction, BMI inhibits conjugated double bonds formation and improves the adhesion between particles and particles, which is beneficial to improvement of final properties. Therefore, BMI improves the mechanical properties of sintered WRP greatly.
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