Browsing by Author "He, S"

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    Iron single atoms on graphene as nonprecious metal catalysts forhHigh‐temperature polymer electrolyte membrane fuel cells
    (Wiley, 2019-03-13) Cheng, Y; He, S; Lu, SF; Veder, JP; Johannessen, B; Thomsen, L; Saunders, MJ; Becker, T; De Marco, R; Li, QF; Yang, SZ; Jiang, SP
    Iron single atom catalysts (Fe SACs) are the best‐known nonprecious metal (NPM) catalysts for the oxygen reduction reaction (ORR) of polymer electrolyte membrane fuel cells (PEMFCs), but their practical application has been constrained by the low Fe SACs loading (<2 wt%). Here, a one‐pot pyrolysis method is reported for the synthesis of iron single atoms on graphene (FeSA‐G) with a high Fe SAC loading of ≈7.7 ± 1.3 wt%. The as‐synthesized FeSA‐G shows an onset potential of 0.950 V and a half‐wave potential of 0.804 V in acid electrolyte for the ORR, similar to that of Pt/C catalysts but with a much higher stability and higher phosphate anion tolerance. High temperature SiO2 nanoparticle‐doped phosphoric acid/polybenzimidazole (PA/PBI/SiO2) composite membrane cells utilizing a FeSA‐G cathode with Fe SAC loading of 0.3 mg cm−2 delivers a peak power density of 325 mW cm−2 at 230 °C, better than 313 mW cm−2 obtained on the cell with a Pt/C cathode at a Pt loading of 1 mg cm−2. The cell with FeSA‐G cathode exhibits superior stability at 230 °C, as compared to that with Pt/C cathode. Our results provide a new approach to developing practical NPM catalysts to replace Pt‐based catalysts for fuel cells. © 1999-2024 John Wiley & Sons, Inc or related companies. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
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    Unsaturated edge-anchored Ni single atoms on porous microwave exfoliated graphene oxide for electrochemical CO2
    (Elsevier, 2019-04) Cheng, Y; Zhao, S; Li, H; He, S; Veder, JP; Johannessen, B; Xiao, J; Lu, S; Pan, J; Chisholm, MF; Yang, SZ; Liu, C; Chen, JG; Jiang, SP
    Supported single atom catalysts (SACs), emerging as a new class of catalytic materials, have been attracting increasing interests. Here we developed a Ni SAC on microwave exfoliated graphene oxide (Ni-N-MEGO) to achieve single atom loading of ∼6.9 wt%, significantly higher than previously reported SACs. The atomically dispersed Ni atoms, stabilized by coordination with nitrogen, were found to be predominantly anchored along the edges of nanopores (< 6 nm) using a combination of X-ray absorption spectroscopy (XAS) and aberration-corrected scanning transmission electron microscopy (AC-STEM). The Ni-N-MEGO exhibits an onset overpotential of 0.18 V, and a current density of 53.6 mA mg−1 at overpotential of 0.59 V for CO2 reduction reaction (CO2RR), representing one of the best non-precious metal SACs reported so far in the literature. Density functional theory (DFT) calculations suggest that the electrochemical CO2-to-CO conversion occurs more readily on the edge-anchored unsaturated nitrogen coordinated Ni single atoms that lead to enhanced activity toward CO2RR. © 2018 Elsevier B.V. All rights reserved.
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    Vortex fluidic induced mass transfer across immiscible phases
    (Royal Society of Chemistry, 2022-01-31) Jellicoe, M; Igder, A; Chuah, C; Jones, DB; Luo, X; Stubbs, KA; Crawley, EM; Pye, SJ; Joseph, N; Vimalananthan, K; Gardner, Z; Harvey, DP; Chen, XJ; Salvemini, F; He, S; Zhang, W; Chalker, JM; Quinton, JS; Tang, YH; Raston, CL
    Mixing immiscible liquids typically requires the use of auxiliary substances including phase transfer catalysts, microgels, surfactants, complex polymers and nano-particles and/or micromixers. Centrifugally separated immiscible liquids of different densities in a 45° tilted rotating tube offer scope for avoiding their use. Micron to submicron size topological flow regimes in the thin films induce high inter-phase mass transfer depending on the nature of the two liquids. A hemispherical base tube creates a Coriolis force as a ‘spinning top’ (ST) topological fluid flow in the less dense liquid which penetrates the denser layer of liquid, delivering liquid from the upper layer through the lower layer to the surface of the tube with the thickness of the layers determined using neutron imaging. Similarly, double helical (DH) topological flow in the less dense liquid, arising from Faraday wave eddy currents twisted by Coriolis forces, impact through the less dense liquid onto the surface of the tube. The lateral dimensions of these topological flows have been determined using ‘molecular drilling’ impacting on a thin layer of polysulfone on the surface of the tube and self-assembly of nanoparticles at the interface of the two liquids. At high rotation speeds, DH flow also occurs in the denser layer, with a critical rotational speed reached resulting in rapid phase demixing of preformed emulsions of two immiscible liquids. ST flow is perturbed relative to double helical flow by changing the shape of the base of the tube while maintaining high mass transfer between phases as demonstrated by circumventing the need for phase transfer catalysts. The findings presented here have implications for overcoming mass transfer limitations at interfaces of liquids, and provide new methods for extractions and separation science, and avoiding the formation of emulsions. © 2022 The Author(s). Published by the Royal Society of Chemistry. Open Access CC BY.