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| 001 | 599477 | ||
| 005 | 20250724132544.0 | ||
| 024 | 7 | _ | |a 10.26434/chemrxiv-2023-jfnmr |2 doi |
| 024 | 7 | _ | |a 10.3204/PUBDB-2023-07449 |2 datacite_doi |
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| 037 | _ | _ | |a PUBDB-2023-07449 |
| 041 | _ | _ | |a English |
| 100 | 1 | _ | |a Li, Yongchun |0 P:(DE-H253)PIP1098115 |b 0 |
| 245 | _ | _ | |a Competing mechanisms determine oxygen redox in doped Ni-Mn based layered oxides for Na-ion batteries |
| 260 | _ | _ | |c 2023 |
| 336 | 7 | _ | |a Preprint |b preprint |m preprint |0 PUB:(DE-HGF)25 |s 1706880155_1861217 |2 PUB:(DE-HGF) |
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| 520 | _ | _ | |a Cation doping is an effective strategy for improving the cyclability of layered oxide cathode materials through suppression of phase transitions in the high voltage region (>~4.0V). In this study we choose Mg and Sc as representative dopants in P2- Na$_{0.67}$Ni$_{0.33}$Mn$_{0.67}$O$_2$. While both dopants have a positive effect on the cycling stability, they are found to influence the properties in the high voltage regime in different ways. Through a combination of RIXS, XRD, XAS, PDF analysis, and DFT, we show that it is more than just suppression of the P2 to O$_2$ phase transition that is critical for promoting the favorable properties, and that the interplay between Ni and O activity are also critical aspects that dictate the performance. With Mg doping, we could enhance the Ni activity while simultaneously suppressing the O activity. This is surprising because it is in contrast to what has been reported in other Mn-based layered oxides where Mg is known to trigger oxygen redox. We address this contradiction by proposing a competing mechanism between Ni and Mg that impacts differences in O activity in Na$_{0.67}$Mg$_x$Ni$_{0.33-x}$Mn$_{0.67}$O$_2$ (x<0<0.33). These findings provide a new direction in understanding the effects of cation doping on the electrochemical behavior of layered oxides. |
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| 700 | 1 | _ | |a Mazzio, Katherine |0 0000-0001-9565-7301 |b 1 |e Corresponding author |
| 700 | 1 | _ | |a Yaqoob, Najma |0 P:(DE-HGF)0 |b 2 |
| 700 | 1 | _ | |a Sun, Yanan |0 P:(DE-H253)PIP1102693 |b 3 |
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| 700 | 1 | _ | |a San Jose Mendez, Alba |0 P:(DE-H253)PIP1080469 |b 8 |u desy |
| 700 | 1 | _ | |a Schuck, Götz |0 P:(DE-HGF)0 |b 9 |
| 700 | 1 | _ | |a Zając, Marcin |0 P:(DE-HGF)0 |b 10 |
| 700 | 1 | _ | |a Kaghazchi, Payam |0 P:(DE-HGF)0 |b 11 |
| 700 | 1 | _ | |a Adelhelm, Philipp |0 P:(DE-H253)PIP1098137 |b 12 |e Corresponding author |
| 773 | _ | _ | |a 10.26434/chemrxiv-2023-jfnmr |
| 856 | 4 | _ | |u https://chemrxiv.org/engage/chemrxiv/article-details/650d854bed7d0eccc30399a3 |
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