JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2021
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IF 2.694
Huijuan Li,Shunguo Qiu,Li Chen,Taotao Fan,Xiong Peng,Zongcheng Yan
A deep eutectic solvent (DES)-based aqueous biphasic system (ABS) denotes a clean and highly biocompatible separation and purification technology, but the explanations of the phase formation mechanism and phase behavior of a DES-based ABS are incomplete. To improve the study of the formation mechanism of a DES-based ABS, a new ABS composed of n-propanol (NPA) and DES with betaine as the hydrogen-bond acceptor (HBA) and polyol as the hydrogen-bond donor (HBD) was formed. The phase formation mechanism of this new ABS and the stability of the DES in the ABS were studied. Betaine and three polyols are hydrophilic (log KOW < 0), whereas NPA is relatively hydrophobic (log KOW > 0). Two phases were formed, because the two components of DES were incompatible with the NPA. The molar ratio of the HBA and HBD in the two phases differed, but in the bottom phase of this ABS, the stoichiometric ratio of HBA and HBD was the same as their initial ratio. Under certain conditions, this novel ABS was considered a ternary-like system. The combination of a series of factors, such as HBD hydrophilicity, molar volume, molecular weight, and initial molar ratio of HBA and HBD, affected the final stoichiometric ratio of HBA and HBD in the top phase.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Hongxia Liu,Hui Mei,Shiping Li,Longkai Pan,Zhipeng Jin,Gangqiang Zhu,Laifei Cheng,Litong Zhang
Bismuth titanate (Bi 12 TiO 20 ) with unique sillenite structure has been shown to be an excellent photocatalyst for environmental remediation. However, the narrow light-responsive range and rapid recombination of photoinduced electrons-holes limit the photocatalytic performance of Bi 12 TiO 20 . To overcome the limitations, a practical and feasible way is to fabricate heterojunctions by combining Bi 12 TiO 20 with suitable photocatalysts. Here, using a facile chemical precipitation method, a novel and hierarchical core–shell structure of n-Bi 12 TiO 20 @p-BiOI (BTO@BiOI) heterojunction was rationally designed and synthesized by loading BiOI nanosheets on BTO nanofibers. The constructed BTO@BiOI composites exhibited significant charge transfer ability due to the synergistic effects of the built-in electric field between BTO and BiOI as well as close interfacial contacts. In addition, the narrow bandgap characteristics of the BiOI led to wide light absorption ranges. Therefore, the BTO@BiOI heterojunction exhibited an improved photocatalytic performance under visible light irradiation. The NO removal efficiency of optimal BTO@BiOI was 45.7%, which was significantly higher compared to that of pure BTO (3.6%) or BiOI (23.1%). Moreover, the cycling experiment revealed that BTO@BiOI composite has a good stability and reusability. The possible mechanism of photocatalytic NO oxidation over BTO@BiOI was investigated in detail.
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SENSORS AND ACTUATORS B-CHEMICAL
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2021
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IF 7.46
Jiaoyan Xu,Mengzhen Lv,Jingjing Yang,Qingxin Chuai,Xiyue Cao,Jianfei Xia,Feifei Zhang,Tingting Zou,Zonghua Wang
In this paper, an exfoliated N-doped honeycomb cavernous carbon (ENC-800) with enhanced properties has been successfully synthesized by exfoliating carbonized metal-organic frameworks with high nitrogen content (N-MOFs) at liquid phase. Due to the high nitrogen content inheriting from the rich-imidazolyl organic ligand, ENC-800 shows excellent electrocatalytical activity and good performance as electrochemical detection platform. The substantial existence of graphitic N in ENC-800 provides generous C-N active site and high conductivity for catalyzing reaction. In addition, the increased specific surface area caused by exfoliation and evaporation of organic solvents confined in the N-MOFs also contributes to the electrochemical performance of ENC-800. In order to explore the potentiality of this material in electrochemical field, chloramphenicol (CAP) was detected by ENC-800 modified electrode and satisfactory results were obtained. In optimized conditions, the linear response of the ENC-800/GCE for CAP was obtained from 0.05 μM to 0.10 mM and from 0.10 mM to 3 mM with detection limit of 0.04 μM. Meanwhile, the new method to obtain an enhanced specific surface area by carbonizing solvent-contained MOFs provides a novel direction for post-processing of MOFs.
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MICROCHIMICA ACTA
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2021
·Vol. 188
·期 10
·1-12
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IF 5.833
Wu Wenrui,Tang Ruizhi,Pan Lei,Wang Chenyang,Zhang Jingjing,Ma Shujuan,Shen Yehua,Ou Junjie
A kind of zwitterionic microsphere was prepared via one-step inverse suspension polymerization employing 3-[ N , N -dimethyl-[2-(2-methylpropyl-2-enyloxy) ethyl] ammonium] propane-1-sulfonate (MSA) and N,N -methylene bisacrylamide (BIS) as the precursors. The preparation conditions were carefully investigated and optimized by regulating the content of total monomers, ratio of MSA to BIS, ratio of water to oil, and content of stabilizer. The properties of microspheres were characterized by helium ion microscopy (HIM), Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), N 2 adsorption/desorption measurement, and water contact angle measurement. The particle size of resulting polydisperse microspheres ranged from 15–25 μm, exhibiting high specific surface area of 138 m 2 g −1 . Owing to great hydrophilicity, the resulting zwitterionic microspheres could be directly used as hydrophilic interaction chromatography (HILIC) sorbent to enrich glycopeptides from biosamples without any chemical modification. A total of 19 N-glycopeptides was enriched from 10 μg of IgG digest. Besides, up to 383 N-glycopeptides and 224 N-glycosylation sites were unambiguously identified from 2 μL of human serum digest by cLC-MS/MS after enrichment with zwitterionic microspheres, indicating their great enrichment performance to N-glycopeptides. The approach of preparing hydrophilic zwitterionic microspheres contains only one synthesis reaction and is suitable for large-scale preparation. Graphical abstract
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SYNTHETIC METALS
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2021
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IF 3.266
Jiaoyan Shi,Lipeng Wu,Qingya Sun,Fan Wu,Aming Xie
Elemetal doping is an efficient strategy to adjust the microstructue and electronic property of a carbon material, as a result, shows great potential in the design of novel electromagnetic absorption (EMA) materials. In this work, we report an useful strategy to prepare a N,S co-doped carbon (NSC) using TTF-TCNQ as the precusor, and systematically explore its frequency-depedent dielectric and EMA properties. Different N/S ratios can be tuned by the regulation of pyrolitic temperature. The derived NSC exhibits wonderful EMA performance when the pyrolytic temperature is setted to 700 ℃ with loading ratio of 35 wt%. Efficient absorption can be achieved in the frequency range of 6.4–18 GHz. Moreover, it is determined that the efficient absorption bandwidth gets to 6.5 GHz, while the maximal absorption reaches −46 dB. The EMA mechanism of NSC is considered to be mainly contributed by improved impedance matching realized by macropores, enhanced conductance loss caused by well constructed condutive network, and polarization by N,S doping. This research provides a new idea for development of novel carbon materials for EMA applicaion.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Yuanyuan Guo,Anrui Dong,Qi Huang,Qipeng Li,Yue Hu,Jinjie Qian,Shaoming Huang
The rational design and preparation of nonprecious metal-based oxygen reduction reaction (ORR) catalysts to facilitate electron and mass transport are of great significance in oxygen-involved energy applications. Herein, a stepwise approach to synthesize a type of hierarchically porous N -doped carbon nanotubes (CNTs) grafted onto zinc-based coordination polymer derived carbon nanomaterials (M−NCNT, M = Fe/Co/Ni) is proposed. At first, an isostructural zinc-based metal–organic framework (MOF) to HKUST-1(Cu) ( ZnHKUST-1 ) is solvothermally prepared, and then under pyrolysis to obtain MOF-derived porous carbon. After the secondary calcination, the in-situ formed N -doped CNTs are efficiently catalyzed by iron group metal-based nanoparticles (Fe/Co/Ni), which are thermally reduced by porous carbon together with additional urea. The synergistic effect between ultrahigh porosity, large surface area, suitable N -doping, high graphitization degree, and ultrafine metal particles prompts M−NCNT series to exhibit satisfactory electrocatalysis in oxygen reduction. Among them, Fe-NCNT owns the optimal ORR activity with high positive onset potential (0.987 V), half-wave potential (0.860 V) and large diffusion-limited current density (4.893 mA cm −2 ). Meanwhile, it shows a high current retention of 90.7% after the 24-hour stability, and the obtained Zn-air battery by Fe-NCNT with open-circuit voltage of 1.44 V owns moderate capacity and satisfying stability. The demonstrated method to prepare hierarchically porous N -doped carbon nanomaterials stemmed from MOF precursors unfolds a new route for the facile construction of efficient nanocatalysts for advanced energy applications.
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Frontiers in Bioengineering and Biotechnology
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2021
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IF 5.89
Lv Xianqing,Yang Guangxu,Gong Zhenggang,Cheng Xin,Shuai Li,Huang Liulian,Chen Lihui,Luo Xiaolin,Liu Jing
Chemical pretreatment followed by enzymatic hydrolysis has been regarded as a viable way to produce fermentable sugars. Phenylsulfonic acid (PSA) pretreatment could efficiently fractionate the non-cellulosic components (hemicelluloses and lignin) from bamboo and result in increased cellulose accessibility that was 10 times that of untreated bamboo. However, deposited lignin could trigger non-productive adsorption to enzymes, which therefore significantly decreased the enzymatic hydrolysis efficiency of PSA-pretreated bamboo substrates. Herein, poly(N-vinylcaprolactam) (PNVCL), a non-ionic surfactant, was developed as a novel additive for overcoming the non-productive adsorption of lignin during enzymatic hydrolysis. PNVCL was found to be not only more effective than those of commonly used lignosulfonate and polyvinyl alcohol for overcoming the negative effect of lignin, but also comparable to the robust Tween 20 and bovine serum albumin additives. A PNVCL loading at 1.2 g/L during enzymatic hydrolysis of PSA pretreated bamboo substrate could achieve an 80% cellulosic enzymatic conversion and meanwhile reduce the cellulase loading by three times as compared to that without additive. Mechanistic investigations indicated that PNVCL could block lignin residues through hydrophobic interactions and the resultant PNVCL coating resisted the adsorption of cellulase via electrostatic repulsion and/or hydration. This practical method can improve the lignocellulosic enzymatic hydrolysis efficiency and thereby increase the productivity and profitability of biorefinery.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Shungui Deng,Xiaotang Shi,Yue Zhao,Chao Wang,Jinghua Wu,Xiayin Yao
Lithium sulfur (Li-S) batteries hold promise as next-generation high energy density devices due to their high theoretical capacities. However, their commercialization confronts great challenges, in particular the notorious shuttle effect and sluggish kinetics, making it difficult to realize high sulfur loading and cell energy density properties. Herein, we explore the potential of molybdenum carbide (Mo 2 C) as the cathode catalyst to promote the polysulfide conversion. Nanosized Mo 2 C embedded porous carbon network (Mo 2 C@PCN) are prepared through the pyrolysis of molybdenum and chitosan precursor. Both electrochemical performance and theoretical calculations reveal that introducing the Mo 2 C can not only enhance the affinity toward the polysulfide intermediate, but also significantly accelerate the polysulfide interconversion compared with that of the pristine porous carbon network (PCN), thereby endowing the Li-S batteries with excellent cycling stability with a low capacity decay of 0.034 % per cycle over 600 cycles, and superb rate capability of 644 mAh g −1 at 5 A g −1 .
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Hongwei Liang,Guanghui Wu,Hongwei Zhang,Qunhong Liu,Qin Yang,Shaohui Xiong,Yuanyuan Yue,Pei Yuan
Mesoporous hollow carbon spheres have been considered as promising adsorbents for volatile organic compounds (VOCs) removal. However, the influence of the morphologies and structures on the adsorption performance of VOCs is still unclear. Herein, we developed a novel strategy for the controllable synthesis of nitrogen-doped mesoporous hollow carbon nanomaterials with adjustable morphologies and structures. By simply tuning tetraethyl orthosilicate addition time and ammonia amount in Stöber system, bowl-like, hollow, and yolk-shell carbon nanomaterials can be obtained. When used as toluene adsorbents, the bowl-like materials exhibited a capacity of 190 mg/g, higher than other carbon materials with different morphologies. The high adsorption capacity and fast adsorption rate of the bowl-like structures can be attributed to the high surface area, rich microporous/mesoporous structure and unique morphology. Our work provides a new strategy for the designed synthesis of novel VOCs adsorbents with advanced adsorption performance.
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SENSORS AND ACTUATORS B-CHEMICAL
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2021
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IF 7.46
Jie Yang,Lu Yang,Xin Tang,Yu Zhang,Qiaoyan Dong,Zhiyuan He,Nihong Li,Ke Huang,Hong Luo,Xiaoli Xiong
As a highly toxic substance that may be harmful to the environment and human beings, hydrazine has been paid growing attention in the field of electrochemical detection . Using the organometallic framework as a template and taking advantage of its high porosity, we prepared cobalt disulfide rhombic dodecahedral nanocomposites with nitrogen coordination and graphene coating (N-CoS 2 @graphene) in this study. Nitrogen coordination can effectively boost the intrinsic activity of the active site by modulating the electronic structure of the Co center in N-CoS 2 @graphene. The surface graphene layers not only work as protective layers to enhance stability but also promote electron transfer. It has been proved that this electrocatalyst has excellent hydrazine electrochemical sensing performance with a high sensitivity of 1580 μA mM −1 cm −2 , a low detection limit of 30 nM at S/N = 3, a linear range from 1.0 μM to 1.0 mM, and satisfactory reproducibility and stability at 0.1 V. It can be seen that this catalyst has a very attractive application prospect in an electrochemical sensor .
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Peng Huang,Peng Zhang,Cuiping Wang,Jingchun Tang,Hongwen Sun
Persulfate-based (PS-based) advanced oxidation process is a promising technology for degradation of organic pollutants . PS activation needs efficient and economical catalysts and heterogeneous Fe-carbon composites are competitive. Herein, novel N-doped biochar-loaded nanoscale zero-valent iron (nZVI) composites (Fe@N-BC) were synthesized and evaluated for PS activation. Detailed characterization data indicated that graphitic and pyridine N structures were introduced by N-doping, which enhanced the anchoring, dispersion and loading of amorphous nZVI on biochar. Remarkably, the optimized Fe@N-BC material, Fe@N 2 -BC 900 , presented excellent catalytic performance for PS activation for lindane removal. The N-doped defects in biochar acted as reactive bridges and accelerated the electron transfer between nZVI and PS, showing strong synergistic effects toward nZVI. O 2 • − and 1 O 2 were the dominant active species in catalytic systems. Additionally, Fe@N 2 -BC 900 catalyst showed effectiveness over a wide pH range for lindane removal. This work provides a new approach to the rational design and application of Fe@N-BC for persulfate activation in pollution control, which is certified by deep exploration of reaction mechanism.
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Nature Communications
·
2021
·Vol. 12
·期 1
·1-9
·
IF 14.919
Zhang Lei,Chen Zhe,Liu Zhenpeng,Bu Jun,Ma Wenxiu,Yan Chen,Bai Rui,Lin Jin,Zhang Qiuyu,Liu Junzhi,Wang Tao,Zhang Jian
Electrocatalytic acetylene semihydrogenation is a promising alternative to thermocatalytic acetylene hydrogenation due to its environmental benignity and economic efficiency, but its performance is far below that of the thermocatalytic reaction because of strong competition from side reactions, including hydrogen evolution, overhydrogenation and carbon–carbon coupling reactions. We develop N–heterocyclic carbene–metal complexes, with electron–rich metal centers owing to the strongly σ–donating N–heterocyclic carbene ligands, as electrocatalysts for selective acetylene semihydrogenation. Experimental and theoretical investigations reveal that the copper sites in N–heterocyclic carbene–copper facilitate the absorption of electrophilic acetylene and the desorption of nucleophilic ethylene, ultimately suppressing the side reactions during electrocatalytic acetylene semihydrogenation, and exhibit superior semihydrogenation performance, with faradaic efficiencies of ≥98 % under pure acetylene flow. Even in a crude ethylene feed containing 1 % acetylene (1 × 10 4 ppm), N–heterocyclic carbene–copper affords a specific selectivity of >99 % during a 100–h stability test, continuous ethylene production with only ~30 ppm acetylene, a large space velocity of up to 9.6 × 10 5 mL·g cat −1 ·h −1 , and a turnover frequency of 2.1 × 10 −2 s −1 , dramatically outperforming currently reported thermocatalysts.
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