| 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. |
- Cichocka, Magdalena Ola, et al.
(författare)
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A Porphyrinic Zirconium Metal-Organic Framework for Oxygen Reduction Reaction : Tailoring the Spacing between Active-Sites through Chain-Based Inorganic Building Units
- 2020
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 142:36, s. 15386-15395
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Tidskriftsartikel (refereegranskat)abstract
- The oxygen reduction reaction (ORR) is central in carbon-neutral energy devices. While platinum group materials have shown high activities for ORR, their practical uses are hampered by concerns over deactivation, slow kinetics, exorbitant cost, and scarce nature reserve. The low cost yet high tunability of metal-organic frameworks (MOFs) provide a unique platform for tailoring their characteristic properties as new electrocatalysts. Herein, we report a new concept of design and present stable Zr-chain-based MOFs as efficient electrocatalysts for ORR. The strategy is based on using Zr-chains to promote high chemical and redox stability and, more importantly, tailor the immobilization and packing of redox active-sites at a density that is ideal to improve the reaction kinetics. The obtained new electrocatalyst, PCN-226, thereby shows high ORR activity. We further demonstrate PCN-226 as a promising electrode material for practical applications in rechargeable Zn-air batteries, with a high peak power density of 133 mW cm(-2). Being one of the very few electrocatalytic MOFs for ORR, this work provides a new concept by designing chain-based structures to enrich the diversity of efficient electrocatalysts and MOFs.
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| 3. |
- 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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| 4. |
- Liang, Zuozhong, et al.
(författare)
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Novel insight into the epitaxial growth mechanism of six-fold symmetrical beta-Co(OH)(2)/Co(OH)F hierarchical hexagrams and their water oxidation activity
- 2018
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Ingår i: Electrochimica Acta. - : Elsevier BV. - 0013-4686 .- 1873-3859. ; 271, s. 526-536
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Tidskriftsartikel (refereegranskat)abstract
- The six-fold symmetry widely presents in both natural and artificial architectures. Understanding the growth mechanism of six-fold symmetrical materials is of fundamental interest and significance. Herein, we report the formation process of beta-Co(OH)(2)/Co(OH)F hierarchical hexagrams with a six-fold symmetrical arrangement. Our results demonstrate that hexagonal beta-Co(OH)(2) plates are first formed under the reaction condition. These hexagonal plates then act as templates for the growth of Co(OH)F nanorods. The intermediate material is therefore composed of plate-like beta-Co(OH)(2) hexagonal cores appended with six rod-like Co(OH)F branches, giving the beta-Co(OH)(2)/Co(OH)F hybrid. After prolonged reaction, the beta-Co(OH)(2) hexagons can be completely converted, leading to authentic six-branched Co(OH)F nanorods as the final product. Consequently, for both intermediate and final materials, the Co(OH)F nanorods are arranged with a six-fold symmetry. Importantly, these Co(OH)F nanorods grow along beta-Co(OH)(2) hexagon edges as lateral branches instead of perpendicular to hexagons. This uncommon epitaxial growth mechanism is considered to be a result of the matching between the b-axis of Co(OH)F crystals and the a-axis of beta-Co(OH)(2) crystals, which is beneficial for the electrocatalysis. The beta-Co(OH)(2)/Co(OH)F hierarchical hexagrams show enhanced water oxidation activity compared to the pure beta-Co(OH)(2) and Co(OH)F.
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| 5. |
- Liang, Zuozhong, et al.
(författare)
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Quasi-single-crystalline CoO hexagrams with abundant defects for highly efficient electrocatalytic water oxidation
- 2018
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Ingår i: Chemical Science. - : Royal Society of Chemistry (RSC). - 2041-6520 .- 2041-6539. ; 9:34, s. 6961-6968
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Tidskriftsartikel (refereegranskat)abstract
- Defects and structural long-range ordering have been recognized as two crucial characters for advanced electrocatalysts. However, these two features have rarely been achieved together. Herein, we report the preparation of single-crystalline CoO hexagrams and demonstrate their exceptional electrocatalytic properties for water oxidation. The quasi-single-crystalline CoO hexagrams, prepared at the critical phase transition point of -Co(OH)(2)/Co(OH)F hexagrams, possess both abundant oxygen vacancies as defects and structural long-range ordering. The matching between the b-axis of Co(OH)F crystals and the a-axis of -Co(OH)(2) crystals is critical for the formation of the CoO hexagram single crystals. The quasi-single-crystalline CoO hexagrams with abundant defects are highly efficient for water oxidation by delivering a 10 mA cm(-2) current density at a low overpotential of 269 mV in a 1 M KOH aqueous solution.
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| 6. |
- Lv, Hao, et al.
(författare)
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Synthesis and Crystal-Phase Engineering of Mesoporous Palladium-Boron Alloy Nanoparticles
- 2020
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Ingår i: ACS central science. - : American Chemical Society (ACS). - 2374-7943 .- 2374-7951. ; 6:12, s. 2347-2353
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Tidskriftsartikel (refereegranskat)abstract
- Rational design and synthesis of noble metal nanomaterials with desired crystal phases (atomic level) and controllable structures/morphologies (mesoscopic level) are paramount for modulating their physiochemical properties. However, it is challenging to simultaneously explore atomic crystal-phase structures and ordered mesoscopic morphologies. Here, we report a simple synergistic templating strategy for the preparation of palladium-boron (Pd-B) nanoparticles with precisely controllable crystal-phases and highly ordered mesostructures. The engineering of crystal-phase structures at atomic levels is achieved by interstitially inserting metallic B atoms into face-centered cubic mesoporous Pd (fcc-mesoPd) confined in a mesoporous silica template. With the gradual insertion of B atoms, fcc-mesoPd is transformed into fcc-mesoPd(5)B, hcp-mesoPd(2)B with randomly distributed B atoms (hcp-mesoPd(2)B-r), and hcp-mesoPd(2)B with an atomically ordered B sequence (hcp-mesoPd(2)B-o) while preserving well-defined mesostructures. This synergistic templating strategy can be extended to engineer crystal-phase structures with various mesostructures/morphologies, including nanoparticles, nanobundles, and nanorods. Moreover, we investigate the crystal-phase-dependent catalytic performance toward the reduction reaction of p-nitrophenol and find that hcp-mesoPd(2)B-o displays much better catalytic activity. This work thus paves a new way for the synthesis of hcp-Pd2B nanomaterials with mesoscopically ordered structure/morphology and offers new insights of fcc-to-hcp evolution mechanisms which could be applied on other noble metal-based nanomaterials for various targeted applications.
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| 7. |
- 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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| 8. |
- Wang, Yanzhi, et al.
(författare)
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Two-Dimensional Metal-Organic Frameworks with Unique Oriented Layers for Oxygen Reduction Reaction : Tailoring the Activity through Exposed Crystal Facets
- 2022
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Ingår i: CCS CHEMISTRY. - : Chinese Chemical Society. - 2096-5745. ; 4:5, s. 1633-1642
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Tidskriftsartikel (refereegranskat)abstract
- As one of the most important families of porous materials, metal-organic frameworks (MOFs) have well-defined atomic structures. This provides ideal models for investigating and understanding the relationships between structures and catalytic activities at the molecular level. However, the active sites on the edges of two-dimensional (2D) MOFs have rarely been studied, as they are less exposed to the surfaces. Here, for the first time, we synthesized and observed that the 2D layers could align perpendicular to the surface of a 2D zeolitic imidazolate framework L (ZIF-L) with a leaf-like morphology. Owing to this unique orientation, the active sites on the edges of the 2D crystal structure could mostly be exposed to the surfaces. Interestingly, when another layer of ZIF-L-Co was grown heteroepitaxially onto ZIF-L-Zn (ZIF-L-Zn@ZIF-L-Co), the two layers shared a common b axis but rotated by 90 degrees in the ac plane. This demonstrated that we could control exposed facets of the 2D MOFs. The ZIF-L-Co with more exposed edge active sites exhibited high electrocatalytic activity for oxygen reduction reaction. This work provides a new concept of designing unique oriented layers in 2D MOFs to expose more edge-active sites for efficient electrocatalysis. [GRAPHICS] .
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| 9. |
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