MICROCHEMICAL JOURNAL
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2021
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IF 4.821
Liya Zhou,Xitong Zhou,Congli Zhao,Yihang Liu,Yaoxuan Li,Li Ma,Ying He,Yanjun Jiang,Jing Gao
Molybdenum carbide (Mo 2 C) doping nitrogen nanoparticles (Mo 2 C/NCS) were synthesized by a facile and friendly method. Owing to the high surface area and structural tunability, Mo 2 C/NCS possesses the excellent electron conduction channels and exposes numerous active sites. Based on these characteristics, Mo 2 C/NCS was adopted to fabricate glassy carbon electrodes to construct acetylcholinesterase (AChE) biosensors for detecting organophosphorus pesticides (OPs). The prepared biosensors exhibited wide linear ranges from 1.0 × 10 −14 to 1.0 × 10 −6 M with the detection limit of 4.47 × 10 −15 M for malathion and 1.0 × 10 −13 to 1.0 × 10 −5 M with a limit of detection of 2.57 × 10 −14 M for methyl paraoxon. The AChE biosensor also displayed the outstanding stability and selectivity. The prepared AChE biosensor was also employed to detect OPs in cabbage and apple samples with high accuracies and satisfactory recoveries. Therefore, this study manifested a prominent transition metal carbides nanomaterial for biosensors in detecting OPs and provided a way for other enzyme-based biosensors.
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JOURNAL OF MATERIALS RESEARCH
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2021
·Vol. 36
·期 6
·1250-1261
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IF 3.089
Lin Zhilan,Zhu Jianhui,Zhang Peixin,Deng Libo
Abstract Spherical carbonaceous materials are considered as ideal electrode materials for supercapacitors because of their high electrical conductivity and excellent electrochemical and mechanical stability. However, their overall performances are yet to be enhanced to meet the future demands. Herein, we prepared a supercapacitive carbon microsphere with hierarchical porous structure and doped them with both nitrogen and phosphor. This was achieved by a facile hydrothermal treatment of cyclodextrin, followed by pyrolysis in the presence of ammonium dihydrogen phosphate and finally by KOH activation. Benefiting from the porous microspheres structure, large surface area, and rich nitrogen and phosphorus heteroatoms, the as-prepared materials demonstrated excellent capacitive performance, with a specific capacitance of 182 F g −1 at 1.0 A g −1 and good rate performance as well as 100% retention after repeated charging and discharging for 5000 cycles, which are superior to the carbon microspheres without heteroatom doping. Graphic abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Xiaoqing Lei,Lijin Huang,Ke Liu,Lei Ouyang,Qin Shuai,Shenghong Hu
Developing high-performance materials for the efficient removal of pharmaceutical contaminants from polluted water has gained tremendous attention but is still a huge challenge. Herein, various N -doped porous carbons (NPCs) were fabricated via a facile and solvent-free pyrolysis strategy by using a mixture of melamine , hexamethylenetetramine , Pluronic F 127, and ZnCl 2 as precursor. The resulting NPCs featuring large specific surface areas (803–1002 m 2 /g) and high nitrogen content (3.79–5.24%) were used as efficient adsorbent for the capture of ibuprofen (IBP) from water. Due to the combination of abundant mesoporous and microporous structure as well as high nitrogen content, the adsorption equilibrium was achieved within 60 min and the adsorption capacity was calculated to be 113 mg/g. Furthermore, it was found that the adsorption capacity exhibited a good correlation with the nitrogen content. In addition, the adsorption capacity of the resulting NPC was well-maintained even after 4 cycles due to its superior stability. The study is expected to encourage the rational design and synthesis of versatile heteroatom-doped porous carbons for practical application in the field of environmental remediation.
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ACS Catalysis
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2021
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IF 13.084
Muhong Li,Shanyong Chen,Qike Jiang,Qingliang Chen,Xuan Wang,Yong Yan,Jian Liu,Changchang Lv,Weiping Ding,Xuefeng Guo
The production of functionalized anilines by chemoselective hydrogenation of nitroarenes occupies an important position in the chemical industries. Recently, cobalt and nitrogen codoped carbon (Co–N–C) catalysts have been reported to show outstanding catalytic performance in this process, whereas the nature of their active sites is still at the center of intense debate. In this paper, based on the well-controlled experiments on four types of typical Co–N–C materials derived from different methodologies, several unusual generalities in the hydrogenation of nitroarenes are clearly revealed, including protic-solvent dependence, antipoisoning, acid resistance, and reversible deactivation. Further investigations indicate that the single-atom species Co–Nx are the main active sites of the Co–N–C catalysts in this chemoselective hydrogenation process. The present work sheds light on the mechanism study on the metal–N–C catalysts and further contributes to the rational design of the high-performance single-atom catalysts.
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JOURNAL OF SUPERCRITICAL FLUIDS
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2021
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IF 4.577
Jian-Lei Qi,Qin-Qin Xu,Dan Zhou,Jian-Zhong Yin,Qi-Ke Jiang
Cu single atoms dispersed on N-doped carbon materials (Cu-NC) were obtained after supercritical CO 2 deposition and decompression, without further post-treatment. AC-HAADF-STEM, STEM , XRD , ICP-OES, and XPS results confirmed that the Cu atoms were equably dispersed over the N-doped carbon (NC) support with the loading of 0.80 wt%. The catalytic performance of Cu-NC in solvent-free oxidation of phenylcarbinol to benzaldehyde was investigated, and the conversion of 73.9% and selectivity of 85.7% were obtained at 50 °C for 1 h. A high-pressure view cell was used to observe the dissolution and diffusion for Cu(acac) 2 in scCO 2 . The stability of Cu-NC structures and the formation path of active oxygen species (O*) on different configurations were predicted by density functional theory (DFT) calculations, and CuN 3 C 1 was found to be more conducive to the activation of tert-butyl hydroperoxide (TBHP).
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TALANTA
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2021
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IF 6.057
Qianying Sheng,Junyan Li,Yingxin Chen,Xinmiao Liang,Minbo Lan
Glycosylation is one of the most important post-translational modifications of proteins, and plays an important role in the structure and function of proteins. However, due to the diversity of glycopeptide forms and their low abundance, it is extraordinarily challenging to capture and separate glycopeptides with high selectivity from complex biological samples with mass spectrometric analysis. Here, we synthesized a new type of hydrophilic composite based on electrostatic interactions , which has been proven to be effective in immobilizing cationic cellulose on graphene oxide-dopamine carriers (expressed as GO-DA-JR), for highly specific enrichment of N-glycopeptides. The introduction of cationic cellulose provides not only a perfect surface charge for the composite but also a greater ability to enrich glycosylated peptides. Thirty-two glycopeptides from human serum immunoglobulin G (IgG) tryptic digests were observed with a greatly improved signal-to-noise ratio (S/N) and also presented high performance in anti-interfering enrichment of glycopeptides from complex samples containing 100-fold bovine serum albumin tryptic digests. In addition, GO–DA-JR has higher sensitivity (1 fmol/μL IgG) and better enrichment capacity (up to 150 mg/g). Moreover, the results of glycopeptide enrichment and glycosylation analysis from human serum also show egood enrichment selectivity from real biological samples. This work exhibits high selectivity, high sensitivity, good stability and operability, indicating its potential for applications of glycopeptides enrichment in post-translational modification proteomics.
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ACS Sustainable Chemistry & Engineering
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2020
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IF 7.632
Zhiyan He,Guangxing Yang,Hongjuan Wang,Fengying Dai,Feng Peng,Hao Yu
Metal- and nitrogen-doped carbon materials (Me–N–C) have received intensive scientific interest as single-atom catalysts (SACs) for electro- and thermocatalytic reactions. In this work, the potential of Me–N–C (Me = Co, Fe, Ni)-wrapped carbon nanotubes (CNTs) as support of platinum nanoparticles (Pt NPs) for base-free oxidation of glycerol was investigated. Co-doping of transition metal and nitrogen significantly enhanced the dispersion of Pt, indicating the advantages of the supporting material for noble-metal catalysts. Two-fold improvement of turnover of glycerol was observed over 5Pt/CoNC@CNT compared to 5Pt/CNT under the same reaction conditions. A kinetics study was conducted to understand the role of CoNC as a support of Pt NPs in a wide range of oxygen partial pressure from 0.04 to 0.4 MPa and a range of glycerol concentration from 0.012 to 0.15 wt %. A synergistic effect between Me–N–C, especially Co–N–C, and Pt NPs was revealed. The Co–N–C support facilitated the activation of oxygen and thus enhanced the overall turnover of glycerol oxidation, especially at high glycerol concentrations. This finding suggests a new approach to the high-performance Pt catalysts via introducing SACs as supporting materials that afford auxiliary active sites for the target reaction.
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INTERNATIONAL JOURNAL OF ENERGY RESEARCH
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2020
·Vol. 45
·期 4
·6227-6238
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IF 3.741
Xiangxiang Du,Xuejun Shi,Yanling Li,Kesheng Cao
Summary Herein, N, S-co-doped graphene hydrogel (N/SGH) was first prepared by one-pot feasible hydrothermal approach using thiourea as a dopant for both N and S sources. And then, polyaniline (PANI) was grown on the surface of N, S-co-doped graphene hydrogel via simple adsorption of aniline monomer and in situ polymerization process. The N, S-co-doped graphene/polyaniline (N/SGH/PANI) composite hydrogel was fabricated as a free-standing and binder-free electrode material. Due to the co-doped synergistic effect, the N/SGH electrode exhibited enhanced electrochemical performances. The N/SGH electrode displays a specific capacitance of 130.4 F/g at 0.5 A/g. Compared with pure graphene hydrogel (GH), the specific capacitance of N/SGH and N-doped graphene (NGH) electrodes at 0.5 A/g increased by 53% and 20%, respectively. PANI pseudocapacitor material was introduced to further improve its capacitive performance. The resultant N/SGH/PANI composite electrode could achieve a max specific capacitance of 236.5 F/g at 0.5 A/g. In addition, N/SGH/PANI composite electrode showed stable cycle performance with the capacity retention of 95.1% after 1000 cycles performed at 10 A/g. Those provide a fabrication strategy for the design of high-performance supercapacitors electrode materials.
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Molecular Catalysis
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2020
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IF 3.687
Zhen-Hong He,Yong-Chang Sun,Kuan Wang,Zhong-Yu Wang,Pan-Pan Guo,Chong-Shan Jiang,Man-Qing Yao,Zhu-Hui Li,Zhao-Tie Liu
N -heterocycles with quinoline and tetrahydroquinoline structures are highly important in pharmaceutical and chemical industries, and their highly efficient mutual transformations are vital but still challenging. In the present work, AlN supported redox cobalt catalysts (Co 3 O 4 /AlN and Co/AlN) were prepared, which could achieve the reversible aerobic oxidative dehydrogenation/hydrogenation of N -heterocycles with good performances. The catalytic performances were stem from the strong interaction between Co species with AlN support, which were confirmed by the characterizations of Raman, XPS, UV–vis DRS, and H 2 -TPR etc . Both of the catalysts showed good stabilities and reusabilities for the titled reactions. Besides, the gram-scale experiments achieved with good yields to corresponding products, revealing the present protocol possesses great potential applications in industry. The strategy of using redox Co-based catalyst not only provides a potential catalyst for the reversible hydrogenation/oxidative dehydrogenation reactions but also replenishes methods for constructing of other redox catalyst, especially with AlN as a carrier.
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CATALYSIS COMMUNICATIONS
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2020
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IF 3.612
Pengbo Wang,Qian He,Hao Zhang,Qingdi Sun,Yujie Cheng,Tao Gan,Xiaohui He,Hongbing Ji
Several research studies have been conducted on N -formylation of amines using phenylsilane and CO 2 . However, most of these studies involved tedious processes of catalyst preparation or complex procedures. In the present study, we describe the use of a simple and commercially available ZnO catalyst for selective N -formylation of amines under mild condition. High-yielding N -formylation products with good recyclability and wide substrate scope were obtained, which can promote fine chemical synthesis and CO 2 capture.
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JOURNAL OF CHROMATOGRAPHY A
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2021
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IF 4.759
Huimin Deng,Ying Wang,Jinbang Wang,Shanshan Liu,Yuan Ji,Ziyan Fan,Zhonghao Li,Fei Yang,Zhaoyang Bian,Gangling Tang
N′ -nitrosonornicotine (NNN) is one of the most prevalent and toxic tobacco-specific nitrosoamines. A chiral center at its 2′-position results in R and S enantiomers, the partial double bond character of the N N = O group also results in E and Z isomers, therefore, NNN can form a total of four absolute configurations ( E -( R )-NNN, E -( S )-NNN, Z -( R )-NNN, and Z -( S )-NNN). This study investigated the resolution of R/S enantiomers and E/Z isomers of NNN by supercritical fluid chromatography tandem mass spectrometry (SFC-MS/MS). The baseline separation of E / Z -( R,S )-NNN isomers/enantiomers was accomplished through the optimization of chiral columns and co-solvents. Due to the lack of single standard of E / Z isomers, only R -NNN (sum of E -( R )-NNN and Z -( R )-NNN) and S -NNN (sum of E -( S )-NNN and Z -( S )-NNN) were further examined. Through the comprehensive optimization of SFC-MS/MS conditions, R -NNN and S -NNN were separated with a run time of 5 min, the developed method was validated, and its applicability to the determination of NNN enantiomers in burley tobacco samples was demonstrated. This study could be applied to preparative separation of single enantiomer and/or isomer of NNN, and could provide potential benefits to biologic activity studies on these enantiomers and isomers.
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Materials Today Chemistry
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2021
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IF 8.301
J. Zhu,C. Shang,X. Wang,G. Zhou
Phosphorus-based materials as the anode for sodium-ion batteries have drawn extensive attention because of their high theoretical capacity and low insertion potential. Nevertheless, the severe volume variation and low electric conductivity hindered their further practical applications. Herein, a novel Co 2 P/Sn 4 P 3 hybrid encapsulated in carbon nanocubes was fabricated by a coprecipitation method followed by phosphating progress. Accompanying with the N, P codoping and abundant grain boundaries, which facilitates electric transport and provides rich active sites, the as-synthesized Co 2 P/Sn 4 P 3 @C anode delivered a high charge specific capacity of 185.6 mA h g −1 after 400 cycles at the current density of 1000 mA g −1 and outstanding cycling stability with a high capacity retention of 86.9%. Kinetics exploration indicated that the capacity was governed by the surface pseudo-capacitive controlled process due to the abundant defects originated from heteroatom doping and grain boundaries.
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