Journal of Materials Chemistry A
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2021
·Vol. 9
·期 11
·7198-7207
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IF 12.732
Xiaoyong Yu,Lijing Wang,Xin Wang,Hongzhi Liu,Ziyuan Wang,Yixuan Huang,Guoqiang Shan,Weichao Wang,Lingyan Zhu
Supported metal catalysts are widely used for heterogeneous catalytic processes (e.g., Fenton-like reaction), but the mechanisms of interfacial processes are still ambiguous. Herein, unique nanocarbon based catalysts with Co nanoparticles encapsulated in nitrogen (N)-doped graphene (Co@NG) were prepared by calcination of Co based metal–organic frameworks (MOFs), which showed excellent catalytic performance for peroxymonosulfate (PMS) activation. Comprehensive characterization revealed that there were strong interfacial interactions between Co and the NG layer due to the presence of special nitrogen species, especially graphitic-N. Density functional theory calculations suggested that the strong interfacial interactions provided optimal active sites with low adsorption energy (−1.99 eV) for PMS accumulation, which enabled the generation of highly oxidizing NG–PMS* intermediates as evidenced by in situ Raman microscopy. Electrochemical analyses revealed that the interfacial interactions facilitated surface-to-surface electronic communication across atomic interface-bonding (N–Co). Consequently, phenol was quickly degraded by the NG–PMS* via direct oxidation by an anodic-like nonradical process, and reasonable graphitic-N (G-N) content and pore size are important for this process. Phenol at 1 mM was completely removed within only 12 min by Co@NG-900 (which was prepared at 900 °C), with an apparent rate constant 20 times higher than that of pure NG-900. This work sheds new insights on the critical role of interfacial interactions in nonradical PMS activation.
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ACS Applied Energy Materials
·
2021
·
IF 6.024
Kexiang Wang,Tingting You,Ran Yin,Bingbing Fan,Jingwen Liu,Shuang Cui,Haining Chen,Penggang Yin
Carbon-based all-inorganic CsPbI2Br perovskite solar cells (C-PSCs) are regarded as a promising photovoltaic candidate due to their low cost, simple device structure, and high stability. However, their power conversion efficiency (PCE) is still too poor for commercial applications, mainly due to the lack of thick and high-quality CsPbI2Br films with less defects. In this work, three antisolvents are chosen to finely control the crystallization process of the CsPbI2Br film based on pure dimethyl sulfoxide solvent; a 500 nm-thick CsPbI2Br film is fabricated using isopropanol as an antisolvent. Furthermore, excess PbI2 is introduced to not only enhance the crystallinity of the CsPbI2Br film and passivate defects located at grain boundaries but also improve the hole extraction from the n-type CsPbI2Br film to the carbon electrode. Consequently, the PCE of CsPbI2Br C-PSC is dramatically boosted up to 12.78% with small hysteresis, which is among the highest values of all-inorganic C-PSCs. Moreover, the unencapsulated C-PSC demonstrates excellent long-term thermal stability, maintaining 93% of its initial PCE after aging at 85 °C for 600 h in dry air. Our work provides significant guidance for developing low-cost, high-performance, and stable CsPbI2Br C-PSCs.
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Energy & Environmental Materials
·
2021
·Vol. 5
·期 1
·353-359
·
IF 15.122
Xingyang Du,Hanying Zhang,Xuexia Lan,Bin Yuan,Renzong Hu
Silicon monoxide (SiO) has aroused increased attention as one of the most promising anodes for high-energy density Li-ion batteries. To enhance the initial Coulombic efficiencies (ICE) and cycle stability of SiO-based anodes, a new facile composition and electrode design strategy have been adapted to fabricate a SiO–Sn–Co/graphite (G) anode. It achieves a unique structure where tiny milled SiO–Sn–Co particles are dispersed among two graphite layers. In this hybrid electrode, Sn–Co alloys promoted Li + extraction kinetics, and the holistic reversibility of SiO and graphite enhanced the electrical conductivity. The SiO–Sn–Co/G electrode delivered an average ICE of 77.6% and a reversible capacity of 640 mAh g −1 at 800 mA g −1 , and the capacity retention was above 98% after 100 cycles, which was much higher than that of the SiO with an ICE of 55.3% and a capacity retention of 50%. These results indicated that this was reliable method to improve the reversibility and cycle ability of the SiO anode. Furthermore, based on its easy and feasible fabrication process, it may provide a suitable choice to combine other alloy anodes with the graphite anode.
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Journal of Physical Chemistry C
·
2021
·
IF 4.126
Tengteng Li,Qingyan Li,Xin Tang,Zhiliang Chen,Yifan Li,Hongliang Zhao,Silei Wang,Xin Ding,Yating Zhang,Jianquan Yao
The preparation of a high-quality perovskite film is very important for improving the device performance of perovskite photodetectors (PPDs). At present, one of the most commonly used methods to obtain high-quality perovskite films is to regulate the nucleation and crystal growth processes through antisolvent-assisted crystallization. In this work, we employ a low-toxicity antisolvent sec-pentanol (SPA) as a polar auxiliary agent to modify the perovskite films, which can effectively regulate the MAI·PbI2·DMSO intermediate phase because of its moderate polarity, leading to the formation of a uniform and pinhole-free perovskite morphology. As a result, the photoresponsivity reaches 1.06 A/W under an illumination of the 532 nm laser with a power density of 12.74 μW/cm2 at a bias voltage of −2 V, which is the known champion responsivity for vertical PD based on an indium tin oxide glass substrate and with CH3NH3PbI3 as the only photosensitive material. Moreover, we study the effects of chlorobenzene with polarity less than SPA and n-butanol with polarity greater than SPA on perovskite formation and device performance as an antisolvent and find that the crystallization quality of the perovskite film is greatly affected by the polarity of the antisolvent. This work provides a reference for the preparation of high-performance PPDs.
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Analytical Methods
·
2021
·Vol. 13
·期 25
·2871-2877
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IF 2.896
Jie Chen,Yabing Gan,Sai Hong,Guoxing Yin,Li Zhou,Changze Wang,Yuchuan Fu,Haitao Li,Peng Yin
Carbon monoxide (CO), a gaseous signal molecule, plays a crucial role in biological systems. With the aim of unraveling its biological functions, a novel fluorescent probe for sensing CO was rationally designed and synthesized based on a coumarin derivative fluorophore merging tetrahydroquinoxaline unit and five-membered pyrrolidine. This fluorescent probe demonstrated a large Stokes shift (Δλ = 132 nm), high quantum yield, red emission, high sensitivity and selectivity for CO with remarkable fluorescence turn-on. And the detection limit for CORM-3 is as low as 31.2 nM with the linear range of 0–30 μM. More importantly, this novel probe has been successfully applied to the fluorescence imaging of CO in HepG2 cells and zebrafish, providing a useful approach for the further understanding of the physiological and pathological roles of CO in living systems.
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PubMed
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Reaction Kinetics Mechanisms and Catalysis
·
2021
·Vol. 134
·期 2
·777-792
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IF 2.081
Liu Yingxin,Zhang Kaiyue,Zhang Liang,Wang Yun,Wei Zuojun
The selective reductive amination of levulinic acid (LA) into pyrrolidone derivatives is regarded as one of the most promising reactions in the fields of biomass conversion into high value-added chemicals. Herein, we report a one-pot synthesis of N -substituted-5-methyl-2-pyrrolidones by reductive amination of LA/ester with nitriles over several commercial catalysts. Among the catalysts texted, Pd/C was found to be the most efficient for the reductive amination of LA/ester with various nitriles to give high yields of pyrrolidones (up to 92%) under mild reaction conditions (80 °C, 1.6 MPa H 2 , tetrahydrofuran solvent). And the catalyst showed good reusability.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Hui Yong,Shuai Wang,Jiangwei Ma,Kewei Zhang,Dongliang Zhao,Jifan Hu,Yanghuan Zhang
The Mg-based hydrogen storage alloy with multiple platforms is successfully prepared by ball milling Co powder and Mg-RE-Ni precursor alloy, and its hydrogen storage behavior was investigated in detail by XRD , EDS , TEM, PCI , and DSC methods. The ball-milled alloy consists of the main phase Mg, the catalytic phases Mg 2 Ni, Mg 2 Co as well as a small amount of Mg 12 Ce, and convert into the MgH 2 –CeH 2.73 -Mg 2 NiH 4 –Mg 2 CoH 5 composite after hydrogenation. The composite has three PCI platforms corresponding to the reversible de/hydrogenation reaction of Mg/MgH 2 , Mg 2 Ni/Mg 2 NiH 4 and Mg 6 Co 2 H 11 /Mg 2 CoH 5 . Among them, the transformation between Mg 2 Ni and Mg 2 NiH 4 triggers the “spill-over” effect which promote the decomposition of MgH 2 phases and enhances the hydrogen desorption kinetics. Meanwhile, the conversion of the Mg 6 Co 2 H 11 to Mg 2 CoH 5 phase induces the “chain reaction” effect, which leads to preferential nucleation of Mg phase and improves the hydrogen absorption kinetics. Therefore, the Mg-RE-Ni-Co alloy has a double improvement on hydrogen absorption and desorption kinetics. Concretely, the alloy has an optimal hydrogen absorption temperature of 200 °C, at which it can absorb 5.5 wt. % H 2 within 40 s. Under the conditions, the capacity of absorption almost reaches the maximum reversible value (about 5.6 wt. %). Besides, the alloy has a dehydrogenation activation energy of 67.9 kJ/mol and can desorb 5.0 wt. % H 2 within 60 min at the temperature of 260 °C.
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Food & Function
·
2021
·Vol. 12
·期 12
·5551-5562
·
IF 5.396
Mengjie Ma,Han Wang,Yongkai Yuan,Yuanhong Wang,Shuang Yang,Zhihua Lv
The purpose of this study was to investigate the absorption and transport of glycosaminoglycan from Apostichopus japonicus (AHG) and its depolymerized derivatives (DAHG-1, DAHG-2, DAHG-3). The AHG and depolymerized AHGs (DAHGs) were characterized by high-performance gel permeation chromatography (HPGPC), Raman spectroscopy and atomic force microscopy (AFM). The results showed that there was no significant difference of an AHG primary structure and functional groups during the depolymerization. Meanwhile, AFM observation showed that AHG and DAHGs possessed linear structures. In this study, a rapid and sensitive liquid chromatographic post-column derivatization method was used to investigate the absorption of AHG and DAHGs with the Caco-2 cell model, the M cell model and the intestinal recirculating perfusion. It was found that AHG and DAHGs can be absorbed in the intestine, and their transport involved endocytosis.
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PubMed
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Progress in Natural Science-Materials International
·
2021
·
IF 3.607
Yaokun Fu,Zhenmin Ding,Lu Zhang,Hongming Zhang,Wenfeng Wang,Yuan Li,Shumin Han
The application of magnesium hydride (MgH 2 ) is limited due to the high reaction temperature and slow kinetics during dehydrogenation. In order to ameliorate the dehydrogenation property of MgH 2 , MgC 0.5 Co 3 compound with induction and catalytic effects was introduced into the Mg/MgH 2 system via ball-milling and hydriding combustion methods in present study. Compared to the pure MgH 2 , the initial hydrogen desorption temperature of MgH 2 –MgC 0.5 Co 3 composite lowered to 237 °C, decreasing by 141 °C. At 325 °C the MgH 2 –MgC 0.5 Co 3 composite could release 4.38 wt% H 2 within 60 min, which is 4.5 times the capacity of hydrogen released by as milled-MgH 2 . Besides, the hydrogen desorption activation energy of the MgH 2 –MgC 0.5 Co 3 composite was dramatically reduced to 126.7 ± 1.4 kJ/mol. It was observed that MgC 0.5 Co 3 was chemically stable and no chemical transformation occurred after cycling, which not only inhibited the nucleation and growth of composite particles, but also had a positive effect on the hydrogen desorption reaction of MgH 2 due to its catalytic effect. This study may provide references for designing and synthesizing Mg–C–Co alloy compound for the Mg-based hydrogen storage area.
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DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 37
·12870-12878
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IF 4.39
Miao Wang,Ali Saad,Xiaoguang Li,Tao Peng,Qi-Tao Zhang,Mohan Kumar,Wei Zhao
High-performance and cost-effective nonprecious-metal catalysts are essential for the next-generation oxygen evolution reaction (OER). However, the electrocatalysis of the OER during water splitting is often carried out by using noble metal catalysts, such as RuO2 or IrO2 with high-cost and limited stability. Herein, we reported a successful synthesis of a ternary nickel monophosphosulfide (NiPS) compound via a simple solid-state route and further investigated its electrocatalytic performances for water oxidation. It is found that the NiPS electrocatalyst exhibits good OER performance in 1.0 M KOH solution, i.e., achieving a current density of 20 mA cm−2 at an overpotential of 400 mV and a Tafel slope of 126 mV dec−1, comparable to commercial benchmark RuO2. The ternary NiPS electrocatalyst for the OER is superior to its binary counterparts, i.e., Ni2P and NiS. Density functional theory (DFT) calculations combined with ex situ XPS were performed to obtain further insights into the intrinsic catalytic mechanism of NiPS, and their results clearly revealed that the instability of the NiO intermediate during the OH* → O* process and the easy oxidation of the (PS)3− anion favoring the formation of hydroxyl-based species (i.e., Ni(OH)2/NiOOH) on the surface of the catalyst, which plays a crucial role in facilitating the OER activity. Furthermore, we creatively extended this method to the fabrication of heteroatom substituted catalysts and a new quaternary CoNiP2S2 compound was successfully synthesized for the first time in the same way. The structural properties and electrocatalytic performance towards the OER for CoNiP2S2 (e.g., 20 mA cm−2 at 376 mV) are also systematically investigated in this work.
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Bioactive Materials
·
2021
·
IF 14.593
Jin Leng,Ye He,Zhang Yuan,Bailong Tao,Ke Li,Chuanchuan Lin,Kun Xu,Maowen Chen,Liangliang Dai,Xuemin Li,Tony Jun Huang,Kaiyong Cai
Ideal percutaneous titanium implants request both antibacterial ability and soft tissue compatibility. ZnO structure constructed on titanium has been widely proved to be helpful to combat pathogen contamination, but the biosafety of ZnO is always questioned. How to maintain the remarkable antibacterial ability of ZnO and efficiently reduce the corresponding toxicity is still challenging. Herein, a hybrid hydrogel coating was constructed on the fabricated ZnO structure of titanium, and the coating was proved to be enzymatically-degradable when bacteria exist. Then the antibacterial activity of ZnO was presented. When under the normal condition (no bacteria), the hydrogel coating was stable and tightly adhered to titanium. The toxicity of ZnO was reduced, and the viability of fibroblasts was largely improved. More importantly, the hydrogel coating provided a good buffer zone for cell ingrowth and soft tissue integration. The curbed Zn ion release was also proved to be useful to regulate fibroblast responses such as the expression of CTGF and COL-I. These results were also validated by in vivo studies. Therefore, this study proposed a valid self-adaptive strategy for ZnO improvement. Under different conditions, the sample could present different functions, and both the antibacterial ability and soft tissue compatibility were finely preserved.
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SURFACE & COATINGS TECHNOLOGY
·
2020
·
IF 3.784
Ying Zhang,Tengfei Han,Meng Xiao,Yifu Shen
(FeNiCoCrTi 0.5 )C x (x = 3 wt%, 6 wt%, 12 wt%) carbonized high-entropy alloy-based composite coatings , marked as C 3 , C 6 and C 12 , were prepared on 45 steel by laser cladding. The macroscopic morphology, phase, microstructure, hardness and wear resistance of coatings have been investigated systematically. The results indicate that diamond content has a significant influence on the microstructure and mechanical properties of (FeNiCoCrTi 0.5 )C x coating. (FeNiCoCrTi 0.5 )C x coatings, without pores and cracks, are well metallurgically bonded with substrate. The coatings consist of BCC solid solution, Cr 23 C 6 and TiC. The addition of diamond in (FeNiCoCrTi 0.5 )C x coating leads to the instability of BCC solid solution and facilitates the precipitation of carbides , which causes carbides to become coarse and aggregate into large blocks. The hardness of (FeNiCoCrTi 0.5 )C x coatings is much higher than that of the 45 steel, the average hardness of C 12 coating is 4 times the hardness of substrate. Besides, the hardness of (FeNiCoCrTi 0.5 )C x coating increases with the increase of diamond content. Nonetheless, compared to C 6 coating, the C 12 coating shows inferior tribological performance due to the brittleness . It is noteworthy that C 6 coating with outstanding wear resistance has the potential to apply in various fields of machinery industry, marine engineering and aerospace.
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