INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Xinkuai He,Zhousi Hu,Jingjing Yang,Ruqing Guo,Luye Wu
The co-deposition behavior of Co(II) and Mo(VI) in N,N-dimethylformamide and ethylene glycol system is observed. The result implies that Co–Mo co-deposition is typical induced deposition, while containing ordinary deposition process . Mo(VI) species in the system can suppress the reduction of Co(II) and its effect can be improved as the increase of Mo(VI) concentration, however, Co(II) species can promote the reduction of Mo(VI) and the effect can also be improved as the increase of Co(II) concentration. SEM micrographs indicate that all these films exhibit a fibrous surface morphology with a new fluffy microstructure. XRD pattern reveals that the Co–Mo film is a Mo solid solution in Co and its average size of crystalline grain is 9.5 nm. In addition, the electrocatalytic activity for hydrogen evolution reaction (HER) on these Co–Mo films is investigated. These results indicate that its electrocatalytic activity can be improved as Mo content increases from 1.02 to 2.84 wt% and the prepared Co–Mo film with 2.84 wt% Mo presents a high electrocatalytic activity and stability for HER with an overpotential of 81 mV at 10 mA cm −2 .
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Coatings
·
2023
·Vol. 14
·期 1
·28
·
IF 3.4
Yaling Deng,Yu Xu,Lei Nie,Yiyang Huang
The development of coatings with efficient lubrication and load-bearing capacity is an urgent need for artificial joints. Here, we successfully fabricated poly (acrylic acid-co-acrylamide)/polyethyleneimine (P(AA-co-AAm)/PEI) coating on titanium alloy (Ti6Al4V) surface via UV irradiation and thermal treatment technique. The dual crosslinked network structures were composed of a P(AA-co-AAm) network via free radical polymerization and a PAA-co-PEI network via thermal crosslinking of amine and carboxyl groups. The thermally crosslinked P(AA-co-AAm)/PEI coatings exhibit a stable low friction coefficient (approximately 0.022) and exceptionally low wear volume, with a 93.8% and 92.6% reduction, respectively, in comparison to the pristine Ti6Al4V. These thermally crosslinked P(AA-co-AAm)/PEI hydrogel coatings exhibit excellent lubrication and anti-wear properties, providing a strategy for developing novel lubricating coatings in the biomedical field.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 40
·14435-14442
·
IF 4
Qihao Wu,Tao Xie,Li Zhang,Hui Ding,Heju Gao,Jiahui Jiang,Guancheng Xu
To achieve broad commercialization of rechargeable metal–air batteries, the development of non-precious metal-based bi-functional oxygen electrocatalysts is critical. In this study, we prepared N,S co-doped porous carbon materials containing Co9S8 nanoparticles (Co9S8/NSC) through a one-step pyrolysis process. The process involved the pyrolysis of a polydopamine (PDA) coated Co-formic acid framework (Co-FF) derived Co3O4 and thiourea. The improved catalyst Co9S8/NSC-1 exhibited satisfactory long-term durability and superior oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) activity, the half-wave potential (E1/2) of the ORR reached 0.83 V, and the OER overpotential at 10 mA cm−2 (η10) was 300 mV. The zinc–air battery (ZAB) based on Co9S8/NSC-1 assembly had a maximum power density of 102.0 mW cm−2 and the cycle life reached 500 cycles. The material preparation method was simple, environmentally friendly and inexpensive, providing a feasible strategy for the development of non-precious metal-based electrocatalysts.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Hongchao Li,Zihao Zhao,Jieshu Qian,Bingcai Pan
The catalytic activation of peroxymonosulfate (PMS) is under intensive investigation with potentials as an alternative advanced oxidation process (AOP) in wastewater treatment. Among all catalysts examined, Co(II) exhibits the highest reactivity for the activation of PMS, following the conventional Fenton-like mechanism, in which free radicals (i.e., sulfate radicals and hydroxyl radicals) are reckoned as the reactive species. Herein, we report that the primary reactive species (PRS) is proposed to be a Co(II)–PMS complex (Co(II)–OOSO3–), while free radicals and Co(III) species act as the secondary reactive species (SRS) that play a minor role in the Co(II)/PMS process. This Co(II)–OOSO3– exhibits several intriguing properties including ability to conduct both one-electron-transfer and oxygen-atom-transfer reactions with selected molecules, both nucleophilic and electrophilic in nature, and strongly pH-dependent reactivity. This study provides novel insights into the chemical nature of the Co(II)-catalyzed PMS activation process.
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Nano Research
·
2020
·Vol. 14
·期 3
·868-878
·
IF 8.183
Lei Zhao,Tan Yangyang,Zhang Zeyi,Wu Wei,Cheng Niancai,Chen Runzhe,Mu Shichun,Sun Xueliang
The construction and design of highly efficient and inexpensive bifunctional oxygen electrocatalysts substitute for noble-metal-based catalysts is highly desirable for the development of rechargeable Zn-air battery (ZAB). In this work, a bifunctional oxygen electrocatalysts of based on ultrafine CoFe alloy (4-5 nm) dispersed in defects enriched hollow porous Co-N-doped carbons, made by annealing SiO 2 coated zeolitic imidazolate framework-67 (ZIF-67) encapsulated Fe ions. The hollow porous structure not only exposed the active sites inside ZIF-67, but also provided efficient charge and mass transfer. The strong synergetic coupling among high-density CoFe alloys and Co-N x sites in Co, N-doped carbon species ensures high oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) activity. First-principles simulations reveal that the synergistic promotion effect between CoFe alloy and Co-N site effectively reduced the formation energy of from O* to OH*. The optimized CoFe-Co@PNC exhibits outstanding electrocatalytic stability and activity with the overpotential of only 320 mV for OER at 10 mA·cm −2 and the half-wave potential of 0.887 V for ORR, outperforming that of most recent reported bifunctional electrocatalysts. A rechargeable ZAB constructed with CoFe-Co@PNC as the air cathode displays long-term cyclability for over 200 h and high power density (152.8 mW·cm −2 ). Flexible solid-state ZAB with our CoFe-Co@PNC as the air cathode possesses a high open circuit potential (OCP) up to 1.46 V as well as good bending flexibility. This universal structure design provides an attractive and instructive model for the application of nanomaterials derived from MOF in the field of sustainable flexible energy applications device.
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Materials Today Energy
·
2020
·
IF 5.604
C. Xu,J. Zhan,Z. Wang,X. Fang,J. Chen,F. Liang,H. Zhao,Y. Lei
Na–CO 2 batteries are prospective in energy storage and CO 2 recycling applications; development of a high-efficiency, low-cost electrocatalyst to promote CO 2 reduction and carbonate decomposition is extremely vital for practical Na–CO 2 batteries. Herein, a highly efficient cathode catalyst for rechargeable hybrid Na–CO 2 batteries is successfully synthesized by encapsulating highly dispersed Co/Co 9 S 8 nanoparticles into carbon skeletons, consisting of biomass-derived S, N-co-doped hierarchically porous carbon (Co/Co 9 S 8 @SNHC). The conductive and hierarchically porous framework structure of the Co/Co 9 S 8 @SNHC can not only accelerate electron transport , electrolyte infiltration , and CO 2 diffusion but also can inhibit overgrowth and agglomeration of Co/Co 9 S 8 nanoparticles and expose numerous high density of active sites, as well as offer sufficient space to store discharge products. Benefiting from the synergistic effect among S and N dopants , carbon defects, and Co/Co 9 S 8 nanoparticles in robust porous carbon structure, the hybrid Na–CO 2 batteries displayed a low charge overpotential (only ~0.32 V) at 0.2 mA/cm 2 and repeatedly charged and discharged over 200 cycles at 0.1 mA/cm 2 . Besides, an ultrahigh areal capacity of ~18.9 mAh/cm 2 was obtained at 0.5 mA/cm 2 , the highest value to date for Na–CO 2 batteries. Meanwhile, the hybrid Na–CO 2 battery charging from Na 2 CO 3 @C catalytic cathode demonstrated the high catalytic activity of biomass-derived S,N-co-doped hierarchically porous carbon (Co/Co 9 S 8 @SNHC) for CO 2 reduction and carbonate decomposition. Given this finding, this work might open up a potential avenue for the reasonable design of low-cost and highly efficient catalysts for advanced metal-CO 2 batteries systems.
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 11
·5595-5600
·
IF 11.301
Kai Deng,Tianlun Ren,You Xu,Songliang Liu,Zechuan Dai,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
Although recent studies on the hydrogen evolution reaction (HER) have achieved great progress, it remains a great challenge to fabricate highly efficient pH-universal HER electrocatalysts. In this work, we report the facile synthesis of a new class of Rh-based spongy aerogels co-incorporated with transition metal M (M = Co, Ni, and Fe) and boron atoms through a simple and versatile one-pot wet-chemical strategy. Benefiting from the synergetic effect of 3D network-shaped spongy architectures and the electronic interaction between various elements, the optimized RhCoB aerogels exhibit excellent catalytic activity, stability and durability toward the HER in a wide pH range. The successful synthesis of RhMB aerogels will provide guidelines for designing and synthesizing an unprecedented class of transition metal and/or non-metal atom doped metallic materials toward potential catalysis and energy applications.
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Journal of Energy Chemistry
·
2021
·
IF 9.676
Minmin Wang,Min Li,Yilin Zhao,Naiyou Shi,Hui Zhang,Yuxue Zhao,Yaru Zhang,Haoran Zhang,Wenhong Wang,Kaian Sun,Yuan Pan,Shoujie Liu,Houyu Zhu,Wenyue Guo,Yanpeng Li,Yunqi Liu,Chenguang Liu
The development of low-cost, efficient, and high atomic economy electrocatalysts for hydrogen evolution reaction (HER) in the entire pH range for sustainable hydrogen production is of great importance but still challenging. Herein, we synthesize a highly dispersed N-doped carbon frames (NCFs) anchored with Co single atoms (SAs) and Co nanoparticles (NPs) catalyst by a doping-adsorption-pyrolysis strategy for electrocatalytic hydrogen evolution. The Co SAs-Co NPs/NCFs catalyst exhibits an excellent HER activity with small overpotential, low Tafel slope, high turnover frequency as well as remarkable stability. It also exhibits a superior HER performance in the entire pH range. Combining with experimental and theoretical calculation, we find that Co SAs with Co-N 3 coordination structure and Co NPs have a strong interaction for promoting synergistic HER electrocatalytic process. The H 2 O molecule is easily activated and dissociated on Co NPs, while the generated H* is easily adsorbed on Co SAs for HER, which makes the Co SAs-Co NPs/NCFs catalyst exhibit more suitable H adsorption strength and more conducive to the activation and dissociation of H 2 O molecules. This work not only proposes a novel idea for constructing coupling catalyst with atomic-level precision, but also provides strong reference for the development of high-efficiency HER electrocatalysts for practical application.
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DALTON TRANSACTIONS
·
2019
·Vol. 48
·期 48
·17741-17751
·
IF 4.052
Jin Li,Ying Song,Yajuan Wang,Hui Zhang
A series of PdCo alloy nanocluster (NC) catalysts x-PdCor/Co(Mg or Ni)Al-LDH (x: Pd loading, r: Co/Pd molar ratio) were synthesized by immobilizing ultrafine PdCor-PVP NCs on flower-like layered double hydroxide (LDH) supports. The sizes of PdCo alloy NCs of the catalysts can be elaborately tuned in ∼1.6–3.2 nm by both Co/Pd ratios and Pd loadings, and the PdCo NCs are mainly dispersed on the edge sites of LDH nanosheets upon a flower-like morphology. The PdCo bimetallic catalysts 0.81-PdCo0.10/MgAl-LDH (2.6 ± 0.6 nm), 0.86-PdCo0.28/MgAl-LDH (2.3 ± 0.7 nm) and 0.79-PdCo0.54/MgAl-LDH (3.2 ± 0.9 nm) exhibit enhanced activity compared with the monometallic Pd catalyst for Heck coupling of iodobenzene with styrene. Particularly, 0.86-PdCo0.28/MgAl-LDH shows the highest activity, which can be attributed to its smallest PdCo0.28 alloy NCs, and the maximum electron density of the Pd0 center resulted from the electron transfer from Co and the strongest PdCo0.28 NCs – LDH synergistic effect. 0.67-PdCo0.28/CoAl-LDH shows much better activity than those of 0.64-PdCo0.28/NiAl-LDH and 0.86-PdCo0.28/MgAl-LDH. The lowest Pd loading sample 0.01-PdCo0.28/CoAl-LDH (1.6 ± 0.4 nm) shows an ultrahigh turnover frequency of 163 000 h−1 (Pd: 1.9 × 10−5 mol%), which is the highest value obtained so far. Meanwhile, the catalyst shows excellent adaptability for the substrates and can be reused for 12 runs without significant loss of activity. The present work may provide a new idea for the simple and green synthesis of ultrafine Pd-based non-noble bimetallic catalysts for varied catalytic processes.
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ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Lanhua Yi,Fujun Lan,Jinge Li,Caixian Zhao
Photocatalytic water splitting for H2 evolution is appealing for transforming solar energy into clean chemical fuel. This technique generally requires noble metals as H2 evolution cocatalysts to facilitate efficient cleavage of water. Herein, we report a noble-metal-free TiO2 nanobelts composite photocatalyst, in which TiO2 nanobelts are supported by nitrogen-doped graphene coordinated with a single Co atom (Co-NG). The results show that Co-NG is an efficient cocatalytst for the photocatalytic H2 production over TiO2. The optimal amount of Co-NG loading is found to be 3.5 wt %, showing a H2 evolution rate of 677.44 μmol h–1 g–1 under illumination of AM 1.5 G simulated sunlight, which is close to that of platinized TiO2 nanobelts and 2.6 and 31.2 times greater than that of 3.5 wt % NG/TiO2 nanobelts composite and pure TiO2 nanobelts, respectively. The significantly improved photocatalytic activity is ascribed to the remarkable synergistic effect between single-atom Co and N-doped graphene, which serve as effective H+ reduction sites and efficient electron acceptors, respectively. Besides, the Co-NG cocatalyst also effectively retards the recombination of photoinduced charge carriers and leads to a prolonged lifetime of charge pairs. This study reveals that Co-NG is an up-and-coming candidate as cocatalyst for development of cost-effective photocatalysts for efficient solar-driven H2 evolution.
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JOURNAL OF POWER SOURCES
·
2014
·
IF 5.211
Weiya Chen,Yanbo Liu,Ying Ma,Wenxiu Yang
Functionalized TiO 2 (f-TiO 2 ) was synthesized by the atom transfer radical polymerization process and then three types of composite nanofiber membranes including PI/PVdF-HFP (PI/PH, with no nanoparticles contained in PI), TiO 2 @PI/PVdF-HFP (T@PI/PH, with TiO 2 mixed in PI) and f-TiO 2 @PI/PVdF-HFP (f-T@PI/PH, with f-TiO 2 blended in PI) were prepared by bicomponent co-electrospinning technique which could separately maintain the original properties of both PVdF-HFP and PI nanofibers. UV–vis characterization manifested that the modified nanoparticles can provide significant improvements in reducing the particle agglomeration . Morphology, porosity, electrolyte uptake and liquid electrolyte contact angle of all the electrospun separators were investigated, and results showed that the composite separator with 2% f-TiO 2 nanoparticle had smaller fiber diameter , higher porosity, larger electrolyte uptake, smaller contact angle and more excellent thermal dimensional stability. More importantly, the tensile strength of all the composite membranes increased by more than three times after thermal calendering process, which resulted from the several bonded points caused by the fusion of PVdF-HFP component with low melting temperature. Additionally, electrochemical properties of PI/PH, 2% T@PI/PH and 2% f-T@PI/PH composite separators and cycling performances of corresponding batteries were evaluated and 2% f-T@PI/PH composite separator showed better properties than the other two.
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JOURNAL OF SEPARATION SCIENCE
·
2014
·Vol. 37
·期 14
·1826-1833
·
IF 2.594
Dan Liu,Tianbin Zhang,Yechun Cheng,Qiong Jia
A polymer monolith microextraction method coupled with high-performance liquid chromatography was developed for the determination of adenosine triphosphate, adenosine diphosphate, and adenosine monophosphate. The monolithic column was synthesized inside fused-silica capillaries using thermal initiation free-radical polymerization with glycidyl methacrylate as the monomer, ethylene dimethacrylate as the cross-linker, cyclohexanol, and 1-dodecanol as the porogen. N -Methylolacrylamide, an important hydrophilic monomer, was incorporated into the polymerization mixture to enhance the hydrophilicity of the poly(glycidyl methacrylate- co -ethylene dimethacrylate) column. The obtained poly(glycidyl methacrylate- co - N -methylolacrylamide- co -ethylene dimethacrylate) monolith was characterized by scanning electron microscopy, Fourier-transform infrared spectra, and X-ray photoelectron spectroscopy. Optimum conditions for the preconcentration and separation of the target adenosines were also investigated. Under the optimum conditions, we obtained acceptable linearities, low limits of detection, and good relative standard deviations. The developed polymer monolith microextraction with high-performance liquid chromatography method exhibited a good performance with recovery values in the range of 76.9−104.7% when applied to the determination of the adenosines in five royal jelly samples.
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