| 1. |
- Bao, Zijia, et al.
(författare)
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A helical polypyrrole nanotube interwoven zeolitic imidazolate framework and its derivative as an oxygen electrocatalyst
- 2022
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Ingår i: Chemical Communications. - : Royal Society of Chemistry (RSC). - 1359-7345 .- 1364-548X. ; 58:80, s. 11288-11291
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Tidskriftsartikel (refereegranskat)abstract
- A helical polypyrrole nanotube interwoven zeolitic imidazolate framework (ZIF) has been prepared for the first time. After pyrolysis, the helical carbon could act as highly active sites, while the 3D-connected nanoarchitecture contributed to fast charge transfer. The derived carbon material exhibits high activity for the ORR and good performance for a Zn–air battery.
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| 2. |
- Huo, Meiling, et al.
(författare)
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A heteroepitaxially grown two-dimensional metal-organic framework and its derivative for the electrocatalytic oxygen reduction reaction
- 2022
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry (RSC). - 2050-7488 .- 2050-7496. ; 10:19, s. 10408-10416
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Tidskriftsartikel (refereegranskat)abstract
- Two-dimensional (2D) metal–organic frameworks (MOFs) have become a hot topic recently due to their high surface area, larger number of exposed active sites, and improved conductivity. Combining different 2D MOFs could introduce new physical and chemical properties. Here, we have synthesized a heteroepitaxially grown 2D zeolitic imidazolate framework with a leaf-like morphology (ZIF-L). ZIF-L has a layer-by-layer dense structure, which possesses a high content of N and metal ions as active sites. ZIF-L-Co is heteroepitaxially grown on ZIF-L-Zn, while ZIF-L-Zn@ZIF-Co has been successfully prepared. After pyrolysis, the heteroepitaxially grown MOF derived ultra-small Co nanoparticle immobilized nitrogen doped carbon (NC) material (HM-Co@NC) exhibits superior oxygen reduction reaction (ORR) activity (Eonset = 0.998 V, E1/2 = 0.905 V) and better stability than Pt/C, achieving well-qualified assemblies for use in rechargeable Zn–air batteries.
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| 3. |
- Wang, Yang, 1991-, et al.
(författare)
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Interface-induced contraction of core–shell Prussian blue analogues toward hollow Ni-Co-Fe phosphide nanoboxes for efficient oxygen evolution electrocatalysis
- 2023
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Ingår i: Chemical Engineering Journal. - : Elsevier BV. - 1385-8947 .- 1873-3212. ; 451, part 1
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Tidskriftsartikel (refereegranskat)abstract
- Hollow metal phosphides play an important role in electrocatalytic oxygen evolution reaction (OER), but directly phosphatizing solid precursors into well-defined hollow structures and further regulating electronic structures of their derived (oxy)hydroxides for boosting OER performance remain great challenges. Herein, we report hollow Ni-Co-Fe phosphide (Ni-Co-Fe-P) nanoboxes with well-defined interior spaces via a core–shell Prussian blue analogue (PBA)-dependent conversion. Starting from Ni-Co PBA nanocubes, a chemical reduction and decomposition process is utilized to fabricate core–shell Ni-Co@Fe PBA nanocubes based on the lattice matching principle, which are then phosphatized into hollow Ni-Co-Fe-P nanoboxes through an interface-induced contraction process. Thanks to well-designed hollow structures, polymetallic compositions, and doping of carbon, hollow Ni-Co-Fe-P nanobox catalyst shows a remarkable OER activity with a small overpotential of 277 mV at 20 mA cm−2. Notably, this catalyst is also highly stable with only 5 % activity decay over 24 h for the OER. Mechanism studies reveal that the electronic regulation of precatalyst-derived (oxy)hydroxides is the key to boost their OER activity. This work demonstrates a novel and effective protocol for designing polymetallic phosphides with well-defined hollow structures towards various targeted applications.
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| 4. |
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| 5. |
- Ge, Meng, et al.
(författare)
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High-Throughput Electron Diffraction Reveals a Hidden Novel Metal-Organic Framework for Electrocatalysis
- 2021
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Ingår i: Angewandte Chemie International Edition. - : Wiley. - 1433-7851 .- 1521-3773. ; 60:20, s. 11391-11397
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Tidskriftsartikel (refereegranskat)abstract
- Metal-organic frameworks (MOFs) are known for their versatile combination of inorganic building units and organic linkers, which offers immense opportunities in a wide range of applications. However, many MOFs are typically synthesized as multiphasic polycrystalline powders, which are challenging for studies by X-ray diffraction. Therefore, developing new structural characterization techniques is highly desired in order to accelerate discoveries of new materials. Here, we report a high-throughput approach for structural analysis of MOF nano- and sub-microcrystals by three-dimensional electron diffraction (3DED). A new zeolitic-imidazolate framework (ZIF), denoted ZIF-EC1, was first discovered in a trace amount during the study of a known ZIF-CO3-1 material by 3DED. The structures of both ZIFs were solved and refined using 3DED data. ZIF-EC1 has a dense 3D framework structure, which is built by linking mono- and bi-nuclear Zn clusters and 2-methylimidazolates (mIm(-)). With a composition of Zn-3(mIm)(5)(OH), ZIF-EC1 exhibits high N and Zn densities. We show that the N-doped carbon material derived from ZIF-EC1 is a promising electrocatalyst for oxygen reduction reaction (ORR). The discovery of this new MOF and its conversion to an efficient electrocatalyst highlights the power of 3DED in developing new materials and their applications.
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| 6. |
- Ge, Meng, et al.
(författare)
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On the completeness of three-dimensional electron diffraction data for structural analysis of metal-organic frameworks
- 2021
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Ingår i: Faraday discussions. - 1359-6640 .- 1364-5498. ; 231
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Tidskriftsartikel (refereegranskat)abstract
- Three-dimensional electron diffraction (3DED) has been proven as an effective and accurate method for structure determination of nano-sized crystals. In the past decade, the crystal structures of various new complex metal-organic frameworks (MOFs) have been revealed by 3DED, which has been the key to understand their properties. However, due to the design of transmission electron microscopes (TEMs), one drawback of 3DED experiments is the limited tilt range of goniometers, which often leads to incomplete 3DED data, particularly when the crystal symmetry is low. This drawback can be overcome by high throughput data collection using continuous rotation electron diffraction (cRED), where data from a large number of crystals can be collected and merged. Here, we investigate the effects of improving completeness on structural analysis of MOFs. We use ZIF-EC1, a zeolitic imidazolate framework (ZIF), as an example. ZIF-EC1 crystallizes in a monoclinic system with a plate-like morphology. cRED data of ZIF-EC1 with different completeness and resolution were analyzed. The data completeness increased to 92.0% by merging ten datasets. Although the structures could be solved from individual datasets with a completeness as low as 44.5% and refined to a high precision (better than 0.04 angstrom), we demonstrate that a high data completeness could improve the structural model, especially on the electrostatic potential map. We further discuss the strategy adopted during data merging. We also show that ZIF-EC1 doped with cobalt can act as an efficient electrocatalyst for oxygen reduction reactions.
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| 7. |
- Jia, Xiaomin, et al.
(författare)
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Single crystal metal-organic framework constructed by vertically self-pillared nanosheets and its derivative for oriented lithium plating
- 2021
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Ingår i: Cuihuà xuébào. - : Elsevier BV. - 0253-9837 .- 1872-2067. ; 42:9, s. 1553-1560
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Tidskriftsartikel (refereegranskat)abstract
- This vertically self-pillared (VSP) structure extends the application range of traditional porous materials with facile mass/ion transport and enhanced reaction kinetics. Here, we prepare a single crystal metal-organic framework (MOF), employing the ZIF-67 structure as a proof of concept, which is constructed by vertically self-pillared nanosheets (VSP-MOF). We further converted VSP-MOF into VSP-cobalt sulfide (VSP-CoS2) through a sulfidation process. Catalysis plays an important role in almost all battery technologies; for metallic batteries, lithium anodes exhibit a high theoretical specific capacity, low density, and low redox potential. However, during the half-cell reaction (Li++e=Li), uncontrolled dendritic Li penetrates the separator and solid electrolyte interphase layer. When employed as a composite scaffold for lithium metal deposition, there are many advantage to using this framework: 1) the VSP-CoS2 substrate provides a high specific surface area to dissipate the ion flux and mass transfer and acts as a pre-catalyst, 2) the catalytic Co center favors the charge transfer process and preferentially binds the Li+ with the enhanced electrical fields, and 3) the VSP structure guides the metallic propagation along the nanosheet 2D orientation without the protrusive dendrites. All these features enable the VSP structure in metallic batteries with encouraging performances.
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| 8. |
- Wang, Chengdong, et al.
(författare)
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The proto-oncogene transcription factor Ets1 regulates neural crest development through Histone Deacetylase 1 to mediate output of bone morphogenetic protein signaling.
- 2015
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Ingår i: Journal of Biological Chemistry. - 1083-351X. ; 290:36, s. 21925-21938
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Tidskriftsartikel (refereegranskat)abstract
- The neural crest (NC) is a transient, migratory cell population that differentiates into a large variety of tissues including craniofacial cartilage, melanocytes, and peripheral nervous system. NC is initially induced at the border of neural plate and non-neuralectoderm by balanced regulation of multiple signaling pathways, among which an intermediate bone morphogenetic protein (BMP) signaling is essential for NC formation. Ets1, a proto-oncogene playing important roles in tumor invasion, has also been implicated in delamination of NC cells. In this study, we investigated Ets1 function in NC formation using Xenopus. Overexpression of ets1 repressed NC formation through down-regulation of BMP signaling. Moreover, ets1 repressed the BMP-responsive gene id3 that is essential for NC formation. Conversely, overexpression of id3 can partially rescue the phenotype of NC inhibition induced by ectopic ets1. Mechanistically, we found that Ets1 binds to id3 promoter as well as Histone Deacetylase 1 (HDAC1), suggesting that Ets1 recruits HDAC1 to the promoter of id3, thereby inducing Histone deacetylation of the id3 promoter. Thus, our studies indicate that Ets1 regulates NC formation through attenuating BMP signaling epigenetically.
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| 9. |
- Wang, Yanzhi, et al.
(författare)
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Anchoring Fe Species on the Highly Curved Surface of S and N Co-Doped Carbonaceous Nanosprings for Oxygen Electrocatalysis and a Flexible Zinc-Air Battery
- 2024
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Ingår i: Angewandte Chemie International Edition. - 1433-7851 .- 1521-3773. ; 63:7
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Tidskriftsartikel (refereegranskat)abstract
- Oxygen reduction reaction (ORR) is of critical significance in the advancement of fuel cells and zinc-air batteries. The iron-nitrogen (Fe−Nx) sites exhibited exceptional reactivity towards ORR. However, the task of designing and controlling the local structure of Fe species for high ORR activity and stability remains a challenge. Herein, we have achieved successful immobilization of Fe species onto the highly curved surface of S, N co-doped carbonaceous nanosprings (denoted as FeNS/Fe3C@CNS). The induction of this twisted configuration within FeNS/Fe3C@CNS arose from the assembly of chiral templates. For electrocatalytic ORR tests, FeNS/Fe3C@CNS exhibits a half-wave potential (E1/2) of 0.91 V in alkaline medium and a E1/2 of 0.78 V in acidic medium. The Fe single atoms and Fe3C nanoparticles are coexistent and play as active centers within FeNS/Fe3C@CNS. The highly curved surface, coupled with S substitution in the coordination layer, served to reduce the energy barrier for ORR, thereby enhancing the intrinsic catalytic activity of the Fe single-atom sites. We also assembled a wearable flexible Zn-air battery using FeNS/Fe3C@CNS as electrocatalysts. This work provides new insights into the construction of highly curved surfaces within carbon materials, offering high electrocatalytic efficacy and remarkable performance for flexible energy conversion devices.
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| 10. |
- Wang, Yanzhi, et al.
(författare)
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Fe Single-atom Sites in Two-Dimensional Nitrogen-doped Porous Carbon for Electrocatalytic Oxygen Reduction
- 2022
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Ingår i: ChemCatChem. - : Wiley. - 1867-3880 .- 1867-3899. ; 14:14
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Tidskriftsartikel (refereegranskat)abstract
- The development of electrocatalysts for oxygen reduction reaction (ORR) is important for energy conversion devices, such as fuel cells, and metal-air batteries. Here, we have developed a confined space strategy to prepare a two-dimensional (2D) leaf-like nitrogen (N)-containing porous carbon as a single-atom catalyst substrate. ZIF−L materials have been confined in a thin silica layer to regulate the pyrolysis. The obtained Fe single atoms doped N-containing porous carbons (Fe SAs/N−C) maintain the 2D morphology and have Fe single-atom active sites. Correspondingly, Fe SAs/N−C exhibits excellent ORR performance (E1/2 of 0.907 V), which is more positive than those of commercially available Pt/C (0.874 V) and most reported non-noble metal catalysts. The durability test shows that Fe SAs/N−C exhibits good stability during electrocatalytic process. This rational design shows a new strategy to prepare 2D catalyst supports with single-atom active sites.
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