APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Xiaoyu Li,Yujia Han,Yike Huang,Jian Lin,Xiaoli Pan,Ziang Zhao,Yanliang Zhou,Hua Wang,Xiaofeng Yang,Aiqin Wang,Lin Li,Botao Qiao,Xiaodong Wang
Selective methanation of CO (SMET) is promising for deep removal of low-concentration CO in excess H 2 . However, the development of suitable catalysts applied in practical conditions remains a great challenge. Here we report a general strategy to develop highly efficient SMET catalysts by using hydrogenated TiO 2 (H-TiO 2 ) as support. The H-TiO 2 supported Ru catalysts can remove CO to below 10 ppm with greater than 50 % selectivity in a wide temperature range of 200−265 °C, with a good long-term stability. Detailed characterizations including operando spectroscopy and in-situ XPS combined with DFT calculation revealed that the lowered Ru valance on H-TiO 2 strengthens CO adsorption on both metal surface and metal-support interface which improved CO activation and inhibited CO 2 hydrogenation, respectively, leading to enhancement of both activity and selectivity.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
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IF 19.503
Xinyue Ma,Jianjun Du,Hao Sun,Fenghui Ye,Xin Wang,Pengfei Xu,Chuangang Hu,Lipeng Zhang,Dong Liu
Efficient and cost-effective electrocatalysts for CO 2 reduction with high selectivity are desirable but remain challenging. Herein, a low-cost and efficient electrocatalyst composed of boron, nitrogen co-doped mesoporous carbon (BNMC) for CO 2 reduction reaction (CO 2 RR) along with the catalytic mechanism are reported. The resultant BNMC (i.e., BNMC-1000) exhibits good CO 2 RR activity with high Faradaic efficiency (FE, 95%) towards CO at low overpotential (423 mV). It is demonstrated that the codoping of nitrogen and boron atom, and the mesopore structure are favorable to the excellent catalytic activity of CO 2 RR. The doped boron atom cooperate with nitrogen atom could adjust the projected density of states of the carbon active site generating a proper adsorbed energy of *COOH and *CO on the carbon surface. This work offers a basic guide for developing metal-free carbon-based CO 2 RR electrocatalysts with high-performance.
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ACS Applied Materials & Interfaces
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2021
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IF 9.229
Yiwei Han,Yichen Zhang,Shuai Wu,Mohammed Jalalah,Saeed A. Alsareii,Yongmei Yin,Farid A. Harraz,Genxi Li
The structures assembled by peptides have attracted great attention due to their unique physicochemical properties. Moreover, the co-assembly of peptides with additional components can endow the structures with extended functions. In this work, we have explored the co-assembly of peptides and carbon nanodots (CNDs) by taking advantage of their non-covalent binding; thus, the obtained structure may show both the recognition capability of peptides and the catalytic activity of CNDs. Therefore, we have further used the assembled structure for the sensitive analysis of transglutaminase 2 with a low detection limit of 0.25 pg/mL. By simply replacing the peptide sequences or the nanomaterials, the strategy proposed in this work can be developed as a universal model to build the co-assemblies of peptides and nanomaterials, thus leading to their broader applications in biological and biomedical research.
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Energy & Environmental Materials
·
2021
·Vol. 6
·期 1
·e12273
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IF 15.122
Huanhuan Zhang,Ke Zhang,Saima Ashraf,Yanping Fan,Shuyan Guan,Xianli Wu,Yushan Liu,Baozhong Liu,Baojun Li
Boron hydrides release an abundant amount of hydrogen in the presence of a suitable catalyst. Accelerating bimolecular activation kinetics is the key to designing cost-effective catalysts for borohydride hydrolysis. In this study, the bimolecular activation of a polar O–Co–P site demonstrated superior hydrogen-generation kinetics (turnover frequency, TOF = 37 min −1 , 298 K) and low activation energy (41.0 kJ mol −1 ) close to that of noble-metal-based catalysts. Through a combination of experiments and theoretical calculations, it was revealed that the activated dangling oxygen atom in the Co–O precursor effectively replaced via surface-phosphorization because of strong electronic interactions between the dangling oxygen and P atoms. This substitution modulated the local coordination environment and electronegativity around the surface Co sites and formed a new polar O–Co–P active site for optimizing the activation kinetics of ammonia borane and water. This strategy based on bimolecular activation may create new avenues in the field of catalysis.
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Crystals
·
2019
·Vol. 9
·期 9
·477
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IF 2.061
Qian-Jun Deng,Min Chen,Dong-Chu Chen,Chang-Ai Chen
The organic ligand (1-methyl-1H-benzo[d]imidazol-2-yl)methanol (HL) was used to react with CoX2·6H2O (X = Cl and Br) under solvothermal conditions to obtain the complex [Co4(L)6(X)2] (1, X = Cl; 2, X = Br). The butterfly-shaped structure of complex 1 and 2 suggest that Co(II) ions have two different coordinated modes, which are five coordination with O3NX environment and six coordination with O4N2environment. In addition, the electrospray ionization mass spectrometry (ESI-MS) analysis indicated that the ion molecular fragment of highest intensity was [Co4(L)6]2+, and there existed a high nuclear fragment peak of [Co7(L)12]2+. Interestingly, it was basically completely transformed into [Co7(L)12]2+two days later, so those two complexes were relatively stable in CH3OH. Magnetic characterization exhibited that complex 1 and 2 display field-induced single-molecule magnetic behavior, of which the energy hillsUeff/kBwere 28 and 20 K under direct-current field of 0.1 T, respectively.Keywords:tetranuclear;butterfly shaped;mass spectrometric;single-molecule magnet (SMM)
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MICROCHIMICA ACTA
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2020
·Vol. 187
·期 2
·1-8
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IF 6.232
Hou Chuantao,Zhang Xueli,Wang Lei,Zhang Fan,Huang Xiaolian,Wang Zonghua
A freestanding and flexible buckypaper modfied with CoP/Co (CoP/Co-BP) is described. It has a sponge-like nanostructure and is shown to enable improved nonenzymatic sensing of glucose. The CoP/Co-BP was prepared by first depositing a uniform layer of ZIF- 67 crystals on BP, followed by two steps of pyrolysis treatment and phosphidation under an argon atmosphere. The morphology and structure of the material were characterized by scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. The electrochemical properties were investigated by cyclic voltammetry and amperometric response. The amperometric sensor, best operated at 0.45 V (vs. SCE) at pH 13 has a linear range that extends from 0.5 μM to 1.8 mM of glucose, a 0.2 μM detection limit (at S/ N = 3), and a sensitivity of 6427 μA mM −1 cm −2 in alkaline solution. This is mainly attributed to the synergistic effect between the highly active CoP nanostructure and BP which results in excellent conductivity. The uniformly distributed CoP nanoparticles in the network of BP prevent the formation of close-packed structure and facilitate electron transfer. The sensor has good selectivity and excellent long-term stability. It was applied to the determination of glucose in spiked human serum, and satisfactory results were obtained.
Schematic presentation of a freestanding and flexible buckypaper modfied with CoP/Co. It has a sponge-like nanostructure and exhibits improved catalytic activity toward glucose oxidation. This material was used for high-performance electrochemical glucose sensing.
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ACS Biomaterials Science & Engineering
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2019
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IF 4.511
Yanting Liu,Yuanyuan Yang,Yajing Shen
The tubularlike three-dimensional tissue scaffold is an important architecture in biomedical engineering, but its construction remains a big challenge for existing techniques. This work reports the polysaccharide-biomaterial-based tubular microcapsule, which was fabricated by integrating a co-axial flow microfluidic chip and a polyelectrolyte complex technique. First, we fabricate the densely packed coiled calcium alginate hydrogel microfibers as the building block by a co-axial microfluid chip. Then, the densely packed coiled microfibers were coated with a multilayer membrane through layer-by-layer adsorption of alginate and chitosan. After that, the microfibers with an alginate–chitosan–alginate membrane were expanded and transformed into a tubular microcapsule structure by liquefaction. The tubular microcapsule exhibits a selectively permeable property of different-molecular-weight FITC-dextran/bovine serum albumin compared with original calcium alginate microfibers. Moreover, the tubular microcapsule with a liquefied lumen and a thin membrane allows the sustainable release of encapsulants under the alkaline environment. Our research paves an alternative way of manufacturing artificial biological tube architectures having potential applications for transporting and delivering drugs.
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EUROPEAN POLYMER JOURNAL
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2019
·
IF 3.621
Weilong Chen,Kun Wu,Zhencai Qu,Mangeng Lu
It has been known that phonon mean free path along polymer chains is much larger than in transverse directions because weak interaction between polymer chains leads to chain distortion and entanglement. In order to improve intensity of intermolecular interaction, a series of co-polyesters (CPE) containing different content of offset π-π stacking structure in side chains were synthesized by means of polycondensation and transesterification in this work. WAXD patterns unfolded diffraction peak at 2θ of 27.6°, standing for structure of offset π-π stacking. On enlarging intensity of offset π-π stacking interaction, specific heat capacity of CPE increased from 1.140 Jg −1 K −1 to 1.410 Jg −1 K −1 and thermal diffusivity rose from 0.194mm 2 s −1 to 0.245mm 2 s −1 . As a result, CPE sample exhibited excellent thermal conductivity (TC) of 0.381 Wm −1 K −1 , which is around twice that of traditional thermoplastics. Hence offset π-π stacking interaction could strengthen capacity of heat absorption and thermal conduction at the same time, which might be a good candidate for enhancing thermal conductivity of intrinsic polymers. Furthermore, strong π-π interaction in side chains could maintain modulus when temperature is over glass temperature. And the Young modulus grew from 0.14 GPa to 0.44 GPa with the augment of offset π-π stacking structure.
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BIOSENSORS & BIOELECTRONICS
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2019
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IF 9.518
Yongze Xie,Min Zhang,Qianyun Bin,Shilei Xie,Lu'an Guo,Faliang Cheng,Weizhong Lv
The fast and accurate detection of Carcinoembryonic Antigen (CEA) plays an important role in clinical cancer treatment and therapy. An ultrasensitive photoelectrochemical (PEC) immunosensor for the detection of CEA was constructed using CdSe@BiVO 4 co-sensitized TiO 2 nanorods as photoactive materials. TiO 2 nanorods were assembled on the FTO modified electrode to immobilize capture antibodies. With a sandwich immunoassay format, CEA and signal antibodies labelled CdSe@BiVO 4 were introduced in sequence via specific immunoreaction, and the ultrahigh sensitivity of this immunoassay results from the following three aspects. Firstly, the co-sensitization of BiVO 4 and CdSe extends the absorption range of TiO 2 from ultraviolet region to visible light region, which can adequately utilize the light energy; Secondly, the effective matching of energy levels among TiO 2 , CdSe and BiVO 4 accelerates the separation and transfer of photogenerated electron-hole pairs and significantly improves the PEC performance; Finally, the introduced Au evidently expedites the interfacial electron transfer from TiO 2 to FTO electrode, further resulting in noticeably increased photocurrent . Based on multiple signal amplification strategy, a largely linear detection range from 0.01 ng mL −1 to 50 ng mL −1 with a low detection limit (0.5 pg mL −1 ) were obtained. In addition, the prepared immunosensor with attractive properties provides a promising platform for PEC detection.
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Science Bulletin
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2019
·
IF 6.277
Xiang Gao,Li An,Dan Qu,Wenshuai Jiang,Yanxiao Chai,Shaorui Sun,Xingyuan Liu,Zaicheng Sun
Photocatalytic N 2 fixation involves a nitrogen reduction reaction on the surface of the photocatalyst to convert N 2 into ammonia. Currently, the adsorption of N 2 is the limiting step for the N 2 reduction reaction on the surface of the catalyst. Based on the concept of photocatalytic water splitting, the photocatalytic efficiency can be greatly enhanced by introducing a co-catalyst. In this report, we proposed a new strategy, namely, the loading of a NiS co-catalyst on CdS nanorods for photocatalytic N 2 fixation. Theoretical calculation results indicated that N 2 was effectively adsorbed onto the NiS/CdS surface. Temperature programmed desorption studies confirmed that the N 2 molecules preferred to adsorb onto the NiS/CdS surface. Linear sweep voltammetry results revealed that the overpotential of the N 2 reduction reaction was reduced by loading NiS. Furthermore, transient photocurrent and electrochemical impedance spectroscopy indicated that the charge separation was enhanced by introducing NiS. Photocatalytic N 2 fixation was carried out in the presence of the catalyst dispersed in water without any sacrificial agent . As a result, 1.0 wt% NiS/CdS achieved an ammonia production rate of 2.8 and 1.7 mg L −1 for the first hour under full spectrum and visible light ( λ > 420 nm), respectively. The catalyst demonstrated apparent quantum efficiencies of 0.76%, 0.39% and 0.09% at 420, 475 and 520 nm, respectively. This study provides a new method to promote the photocatalytic efficiency of N 2 fixation.
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EUROPEAN POLYMER JOURNAL
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2019
·
IF 3.621
Jian Hao,Huiqing Wei,Chunxiang Lu,Yaodong Liu
Poly(acrylonitrile-co-itaconic acid) (PAI) is the most widely used precursor for making high performance carbon fiber. In this study, we synthesized PAI with various contents of itaconic acid (IA) in the range of 0 to 22 mol%. The addition of IA not only changes acrylonitrile (AN) segment length distribution, but also initiate AN cyclization at a lower temperature. The effects of PAI sequence distribution and initiation mechanisms on PAN cyclization were systematically studied by differential scanning calorimetry, nuclear magnetic resonance, Fourier transform infrared spectroscopy and thermogravimetry. These results show how the AN sequence length and the carboxyl groups in IA affect the cyclization reaction, the formed ladder structures, and carbon yields.
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RENEWABLE ENERGY
·
2019
·
IF 5.439
Qing-Lu Song,Yun-Peng Zhao,Fa-Peng Wu,Guo-Sheng Li,Xing Fan,Rui-Yu Wang,Jing-Pei Cao,Xian-Yong Wei
Low aromaticity and a large number of oxygen-bridged bonds among the aromatic structural units of lignin make it possible to obtain chemicals directly. A novel Co/ [email protected] catalyst with high activity towards hydrogenolysis of lignin-derived aryl ethers was synthesized according to the pyrolysis process of a predesigned ZIF-67. According to the results of characterization by powder X-ray diffraction (XRD), N 2 adsorption-desorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS), Co was reduced by the carbonized organic linker of ZIF-67, and N was doped into the carbon skeleton of the catalyst. The effects of holding time, temperature, and initial H 2 pressure on the catalytic performance of Co/ [email protected] were evaluated in the selective hydrogenolysis of benzyl phenyl ether (BPE). BPE was completely converted and the selectivity of monomer reached to 98.2% under optimized reaction conditions. The C alk -O bond in BPE was first dissociated to form toluene and phenol, and then phenol was rapidly hydrogenated to form cyclohexanol. Furthermore, the Co/ [email protected] catalyst shows high activity for hydroprocessing and selective cleavage of other lignin-derived aryl ethers, including phenylethyl phenyl, diphenyl ether, dibenzyl ether, dinaphthalene ether, guaiacol, anisole and veratrole.
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