RSC Advances
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2019
·Vol. 9
·期 55
·31979-31987
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IF 3.049
Wenbin Wang,Ruidong Xu,Bohao Yu,Xuanbin Wang,Suyang Feng
Electrochemical decomposition of water to produce oxygen (O2) and hydrogen (H2) through an anodic oxygen evolution reaction (OER) and a cathodic hydrogen evolution reaction (HER) is a promising green method for sustainable energy supply. Here, we demonstrate that cauliflower-like S-doped iron microsphere films are materials that can efficiently decompose water as an electrocatalyst for the oxygen evolution reaction. FeSx films are prepared by a simple one-step electrodeposition method and directly grow on copper foam from a deep eutectic solvent, ethaline (mixture of choline chloride and ethylene glycol), as a durable and highly efficient catalyst for the OER in 1.0 M KOH. The prepared FeSx/CF, as an oxygen-evolving anode, shows remarkable catalytic performance toward the OER with a moderate Tafel slope of 105 mV dec−1, and require an overpotential of only 340 mV to drive a geometrical catalytic current density of 10 mA cm−2. In addition, this catalyst also demonstrates strong long-term electrochemical durability. This study provides a simple synthesis route for practical applications of limited transition metal nano catalysts.
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APPLIED SURFACE SCIENCE
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2019
·
IF 5.155
Xiuquan Xu,Songmei Wang,Xiaofeng Yu,Jila Dawa,Dongliang Gui,Ronghui Tang
Photocatalytic inactivation has been proved to be an effective strategy for controlling biohazards. Herein, the novel Ag deposited phosphorus and sulfur co-doped g-C 3 N 4 (PSCN) composites with different Ag content were constructed via a facile calcination combining with biogenic-reduction method for inactivating Escherichia coli ( E. coli ). The detailed characterization results indicated that P and S elements were successfully co-doped into g-C 3 N 4 (CN) lattice and Ag nanoparticles (NPs) were evenly deposited on the surface of PSCN with diameter range of 4–20 nm. The Ag/PSCN at depositing amount of 4 wt% (Ag/PSCN-4) achieved the strongest photocatalytic inactivation along with excellent stability, which could completely inactivate 7.0 log cells of E. coli within 60 min of visible light irradiation. This improved bactericidal performance was mainly attributed to the synergistic effects of P-S co-doped together with Ag deposition, which resulted in the increased visible light utilization, the improved separation and transfer efficiency of photo-induced charge carriers. Moreover, active species trapping experiments revealed that the generated superoxide radicals ( O 2 − ) and holes (h + ) played the significant roles in photocatalytic inactivation process. Our present work presented a promising and environmentally friendly strategy to enhance the photocatalytic capacities of CN based composites for pathogens inactivation.
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CHEMICAL ENGINEERING SCIENCE
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2019
·
IF 3.372
Fang Li,Dennis Y.C. Leung
A heterojunction structure of BiVO 4 coupled with a narrow bandgap photocatalyst Bi 2 S 3 was fabricated forming a composite material with strong capacity in visible light absorption and enhancement in the separation rate of photogenerated charge carriers owing to their suitable band structures. As a result, efficiency of hydrogen production through photoelectrocatalysis is highly enhanced. The morphology and composition of as-prepared sample electrodes are measured through X-Ray Diffraction (XRD), scanning electron microscopy (SEM), high resolution transmission electron microscopy (HR-TEM) and X-ray photoelectron spectroscopy (XPS). The performance of the hybrid nanostructure Bi 2 S 3 /BiVO 4 photoelectrode was found to be related to the growing process of Bi 2 S 3 nanowire during the hydrothermal preparation process. The composited Bi 2 S 3 /BiVO 4 photoanode achieved a photoconversion efficiency of 2.9% which is nearly 3-fold that of the bare BiVO 4 electrode under visible light irradiation, while the hydrogen production was greatly enhanced by nearly 5-fold in the photoelectrocatalytic hydrogen production reaction.
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APPLIED SURFACE SCIENCE
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2020
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IF 6.182
Xianglei Cao,Liugen Zhang,Tingxiang Chen,Chao Feng,Zechang Liu,Ying Qi,Wei Wang,Jide Wang
MOF based CdS-MoS 2 composite had strong photoresponse and rich catalytic sites because of the adjustable morphology and large specific surface area. The CdS-MoS 2 composite was synthesized by using the first synthesized Cd-MOF as the precursor. The hydrogen evolution activity was evaluated under simulated light source. The rate of photocatalytic hydrogen production can improve by 47 times for doping 2.5% (w/w) MoS 2 compare to pure CdS. The catalyst was analyzed by the UV/vis absorption spectra, photoluminescence spectra, time-resolved photoluminescence spectra, transient photocurrent responses, electrochemical impedance spectra, Mott-Schottky test, etc. The results revealed that the CdS-MoS 2 can greatly enhance the separation and transport efficiency of photogenerated carriers, and shift the position of conduction band for the catalyst, resulting significantly improve the production of hydrogen. This work provides a new strategy for manufacturing of photocatalyst by MOFs.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Huiqiang Wang,Jiachen Li,Ning Ding,Xianhai Zeng,Xing Tang,Yong Sun,Tingzhou Lei,Lu Lin
The eco-friendly sodium carboxymethylcellulose (CMC-Na)/polyvinyl alcohol (PVA) hydrogel reinforced with cellulose nanocrystal (CNC) and graphitic-like carbon nitride (g-C 3 N 4 ) was firstly prepared as smart adsorption hydrogel with mechanical, thermal and swelling response. Encouragingly, the mechanical properties of the g-C 3 N 4 /CNCs-H hydrogel were enhanced with simply changing the content of g-C 3 N 4 . The 1.0% g-C 3 N 4 /CNCs-H hydrogel had outstanding tensile strength (up to 648 KPa), excellent elongation (1169%) and satisfactory toughness (340 KJ/m 3 ). These enhancements were due to the inherently superior properties of the prepared CMC-Na/PVA and the synergistic effect of strong hydrogen bonding interactions between g-C 3 N 4 , CNCs and CMC-Na/PVA chains. The as-prepared g-C 3 N 4 /CNCs-H hydrogel has high equilibrium swelling capacity (90.47–117.3 g/g), which greatly improved the adsorption capacity of methylene blue (MB, q e > 198.6 mg/g). The adsorption properties of MB on the as-prepared hydrogel fitted well with the pseudo-second-order kinetic model and the Langmuir isotherm model. It was showed that the interaction of π-π stacking and hydrogen bonds resulted in the high adsorption capacity of the hydrogels. This study presented a basis and demonstration for the application of hydrogels in contaminants removal in poisonous waterbodies.
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Entropy
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2019
·Vol. 21
·期 11
·1032
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IF 2.419
Yang Gao,Baohua Guo,Jun Xu
The critical size of the secondary nuclei plays an important role in determining the crystal growth rate. In the past, the Nucleation Theorem has been applied to determine the number of molecules in the critical nuclei of a single-component crystal via variation of the crystal growth rate with dilution by the non-crystallizable component. In this work, we extend the method to the three-component co-crystal poly (ethylene oxide)/urea/thiourea inclusion compound. The theoretical crystal growth kinetics were deduced and the dependence of the radial growth rate of the inclusion compound spherulites on the mass fraction of urea in urea/thiourea was measured. The results reveal that the secondary nuclei of the poly (ethylene oxide)/urea/thiourea inclusion compound consist mainly of ethylene oxide repeating units and urea molecules. We propose that only urea molecules and ethylene oxide repeating units are selected to form the secondary nuclei while co-crystallization of the three components happens at the lateral spreading stage. As a result, the composition of the critical secondary nuclei is different from that of the bulk inclusion compound crystals. The work is expected to deepen our understanding of the nucleation of multi-component co-crystals.Keywords:critical size of nuclei;secondary nuclei;co-crystal;inclusion compound;selective nucleation
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ACS Applied Energy Materials
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2019
·
IF 0
Yongkun Liu,Guohua Jiang,Zheng Huang,Qiuling Lu,Bo Yu,Uwamahoro Evariste,Pianpian Ma
In this paper, seasame-ball-like core–shell hollow mesoporous carbon spheres decorated by NiCo2S4 nanoparticles (NiCo2S4/HMCSs) were prepared via a hydrothermal method. The obtained NiCo2S4/HMCSs could be used as the positive electrodes for asymmetric supercapacitors (ASCs), combining the outstanding electroconductivity of carbonic materials and high capacity of NiCo2S4 nanoparticles. The morphology and structure properties of the obtained NiCo2S4/HMCSs were characterized. The electrochemical properties of the as-obtained composites were characterized by an electrochemical workstation, showing an outstanding capacity of 1098.5 F g–1. Finally, ASCs were further fabricated by using the NiCo2S4/HMCSs as the cathode and hollow mesoporous carbon spheres (HMCSs) as the anode. Moreover, the assembled ASCs exhibited a good energy density of 35.1 Wh kg–1 at a moderate power density of about 203.5 W kg–1 and good cycle ability of ∼90% even after 3000 cycles.
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ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Ying Zhao,Jia Zhao,Qing Li,Chuantao Gu,Boying Zhang,Caihong Liu,Zheng Li,Shuozhen Hu,Shanlin Qiao
It is still a great challenge to design a simple, low-cost and highly active catalyst for the industrial production of hydrogen from water electrolysis. Herein, we report a synthesis of molybdenum disulphide (MoS 2 ) supported on carbon supports with high concentration of doped-nitrogen derived from large scale industrial waste plastics, i.e. melamine (CWM) and polyurethane (CWPU), by a simple hydrothermal reaction . Few layers of MoS 2 nanosheets with high catalytic activity can be very-well dispersed on CWM and CWPU. The supports with high‒nitrogen content can not only greatly improve the conductivity of supported MoS 2 nanosheets, but also provide additional active sites with the presence of high pyridinic‒N content. The synergistic effects between the MoS 2 nanosheet and CWM and CWPU contribute to high hydrogen evolution reaction (HER) activity. As the concentration of doped-N increases, the HER performance of MoS 2 -based catalysts is improved. MoS 2 /CWM 1:1 with the highest nitrogen content (11.1 wt %) shows the lowest overpotential of 56 mV at 10 mA cm −2 , the smallest Tafel slope of 36.6 mV·dec −1 , and the highest exchange current density of 0.35 mA cm −2 in acidic condition, which are comparable to that of commercial 20% Pt/C.
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RSC Advances
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2019
·Vol. 9
·期 6
·2997-3003
·
IF 3.049
Shuaihui Li,Yashen Ma,Yongkang Liu,Gu Xin,Minghua Wang,Zhihong Zhang,Zhongyi Liu
A three dimensional (3D) nanostructured composite based on the self-assembly of MoS2 nanospheres and polyaniline (PANI) loaded on reduced graphene oxide (denoted by 3D MoS2-PANI/rGO) was prepared via a feasible one-pot hydrothermal process. The 3D MoS2-PANI/rGO nanocomposite not only exhibits good functionality and bioaffinity but also displays high electrochemical catalytic activity. As such, the developed 3D MoS2-PANI/rGO nanocomposite can be employed as the sensing platform for simultaneously detecting small biomolecules, i.e., ascorbic acid (AA), dopamine (DA), and uric acid (UA). The peak currents obtained from the differential pulse voltammetry (DPV) measurements depended linearly on the concentrations in the wide range from 50 μM to 8.0 mM, 5.0 to 500 μM, and 1.0 to 500 μM, giving low detection limits of 22.20, 0.70, and 0.36 μM for AA, DA, and UA, respectively. Furthermore, the 3D MoS2-PANI/rGO-based electrochemical sensor also exhibited high selectivity, good reproducibility and stability toward small molecule detection. The present sensing strategy based on 3D MoS2-PANI/rGO suggests a good reliability in the trace determination of electroactive biomolecules.
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ACS Sustainable Chemistry & Engineering
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2019
·
IF 6.97
Mengmeng Shao,Yangfan Shao,Shengjie Ding,Rui Tong,Xiongwei Zhong,Lingmin Yao,Weng Fai Ip,Baomin Xu,Xing-Qiang Shi,Yi-Yang Sun,Xuesen Wang,Hui Pan
Searching photocatalysts for efficient hydrogen production has been a challenging issue for solar-energy harvesting. Using co-catalyst is proven to be an effective approach to improve the efficiency of photocatalyst in water-splitting. Here, we report that carbonized MoS2 (MoS2/Mo2C) can be a superactive co-catalyst in solar-driven hydrogen production. We show that MoS2/Mo2C decorated CdS achieves a high photocatalytic hydrogen evolution rate (34 mmol/h/g, ∼112 times higher than pure CdS) and excellent apparent quantum efficiency (41.4% at 420 nm). The outstanding photocatalytic performance of MoS2/Mo2C/CdS is attributed to the metallic characteristic of MoS2/Mo2C and suitable Gibbs free energy of hydrogen adsorption, leading to enhanced light absorption, fast separation and transportation of photoinduced carriers, and optimal activity in hydrogen evolution reaction (HER). We further show that MoS2/Mo2C as co-catalyst can also dramatically improve the photocatalytic activity of g-C3N4. Our findings demonstrate that the carbonized transition metal disulfide can be active as co-catalyst in photocatalysis, providing guidance on exploring novel photocatalysts for energy harvesting.
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高影响因子
ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Tariq Ali,Xianfu Wang,Kai Tang,Qun Li,Saman Sajjad,Shahid Khan,Sidra Anis Farooqi,Chenglin Yan
Electrocatalytic active sites along the Mo-terminated edge of molybdenum disulfide (MoS 2 ) are responsible for the promising hydrogen evolution reaction (HER) activity but poor electrical convey, and scarcity of active sites may inhibit its electrocatalytic performance. Therefore, enhancing the electronic conductivity and increasing the active sites in basal plane are required to realize more efficient hydrogen evolution activity for layered MoS 2 . Herein, by the incorporation of heterophase SnS 2 quantum dots into the basal plane to form atomic-level heterostructure, we dramatically report the enhanced HER activity from MoS 2 with current density of −10 mA cm −2 at a lowered overpotential of 240 mV, a reduced Tafel slope of 65 mV/dec and a long-term durability over 18 h operation. Structural characterization and electrochemical studies reveal the incorporation of heterophase SnS 2 quantum dots can efficaciously realize the disorder engineering in the atomic level to regulate the electronic structure, optimize the energy barrier of hydrogen adsorption/desorption, and proliferate the catalytic active sites density, thus activating the basal plane of MoS 2 for hydrogen evolution. Density functional theory (DFT) calculation reveals the inception of the improved electrocatalytic activity stemmed from an astronomically immense reduction of the kinetic energy barrier of hydrogen adsorption on and desorption from sulfur sites and sulfur vacancies in the basal plane upon SnS 2 incorporation and Sn doping. Our work engenders an efficient method to active the basal plane of 2H-MoS 2 by the incorporation of SnS 2 heterophase into the atomic layer inducing atomic dislocation and electronic structure optimization.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
IF 14.229
Riyue Ge,Wenxian Li,Juanjuan Huo,Ting Liao,Ningyan Cheng,Yi Du,Mingyuan Zhu,Ying Li,Jiujun Zhang
Efficient photo-electrocatalysts for hydrogen evolution reaction (HER) are synthesized using a facile one-step hydrothermal method. With metal-ion bridges, highly dispersed molybdenum disulfide (MoS 2 ) nanolayers are vertically grown on the reduced graphene oxide (RGO) to form RGO-M-MoS 2 photocatalysts for HER, where M = Fe 3+ , Co 2+ , Ni 2+ , Cu 2+ and Zn 2+ . The results show that the cross-bridging ions can modulate the MoS 2 growth priority and act as efficient charge transfer channels between RGO and MoS 2 , and combine the advantages of the high conductivity of graphene with the photo-electrochemical activity of MoS 2 . The metal-ion bridged MoS 2 -M-RGO heterostructures demonstrate superior catalytic activity toward hydrogen evolution reaction in acid medium, evidenced by the remarkable higher catalytic current density at low overpotential compared with that of MoS 2 -RGO without metal-ion bridge. This study provides a novel and facile route for establishing efficient composite photo-electrocatalysts for water splitting to generate hydrogen.
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