06-wiley-low-body-ratio

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Abstract chars: 1381

Anionic redox chemistry enables extraordinary capacity for Li- and Mn-rich layered oxides (LMROs) cathodes. Unfortunately, irreversible surface oxygen evolution evokes the pernicious phase transition, structural deterioration, and severe electrode-electrolyte interface side reaction with element dissolution, resulting in fast capacity and voltage fading of LMROs during cycling and hindering its commercialization. Herein, a redox couple strategy is proposed by utilizing copper phthalocyanine (CuPc) to address the irreversibility of anionic redox. The Cu-N synergistic effect of CuPc could not only inhibit surface oxygen evolution by reducing the peroxide ion O 2 2 -back to lattice oxygen O 2 -, but also enhance the reaction activity and reversibility of anionic redox in bulk to achieve a higher capacity and cycling stability. Moreover, the CuPc strategy suppresses the interface side reaction and induces the forming of a uniform and robust LiF-rich cathode electrolyte, interphase (CEI) to significantly eliminate transition metal dissolution. As a result, the CuPc-enhanced LMRO cathode shows superb cycling performance with a capacity retention of 95.0% after 500 long-term cycles. This study sheds light on the great effect of N-based redox couple to regulate anionic redox behavior and promote the development of high energy density and high stability LMROs cathode.

Sections

• 1. Introduction (4586 chars)
• 2. Results and Discussion (306 chars)
• 3. Conclusion (1562 chars)
• 4. Experimental Section (4583 chars)

Low Coverage Blocks

• p2 back_matter coverage=0.005: Supporting Information) further confirm that the lattice param- eters of LMRO and LMRO@7CuPc electrodes keep well, indi- cating preparation process does not damage the bulk structure. Figure 1a–c shows the high-angle annular dark field-scanning transmission elec
• p2 scientific_body coverage=0.0: with a retention of 85.6%. Whereas, LMRO@7CuPc shows more steady cycling and remains at a capacity of 264.6 mAh g−1 with a retention of 91.8% compared to the maximum capacity of the eighth cycle, indicating excellent cycling stability. The long-term cycling pe
• p3 scientific_body coverage=0.013: vious that LMRO electrode shows extremely fast capacity fad- ing from 214.2 to 119.6 mAh g−1, with a poor retention of only 55.8% after 500 cycles, and the discharge curves (Figure 2d) show severe voltage decay with a voltage retention of 73.9%, indicat- ing t
• p3 scientific_body coverage=0.008: doping is considered to be an effective method for stabilizing the structure of close-packed oxygen and improving the local elec- tronic structure, and it can effectively suppress voltage decay in LMRO.[47–49] Benefiting from improved capacity and voltage cy- cli
• p3 scientific_body coverage=0.0: phthalocyanine (FePc) and zinc phthalocyanine (ZnPc). All the additives are added into LMRO and the electrode preparation are same as CuPc enhanced electrodes, and the correspond- ing electrochemical performance data are shown in Figures S4 and S5 and Table S4
• p5 scientific_body coverage=0.006: and N ensures the high reaction activity of N element to reduce O2 2−of LMRO in time, and the effect of Cu is also maintained in the next cycling (Figure S7, Supporting Information), thus real- izing the high performance of CuPc redox couple. Operando differenti
• p5 scientific_body coverage=0.0: ratio with a maximum of 30.84% and full O2 2−is reduced back when discharging to 2.0 V, and the investigation on the second cycle also shows the same pattern (Figure S10, Supporting Infor- mation). The above results verify the enhancement of oxygen re- action
• p7 scientific_body coverage=0.0: The better structure stability is also proven by surface-sensitive Raman spectrometry as shown in Figure S12 (Supporting Infor- mation). For the pristine LMRO electrode, the peak located at 415 cm−1 is ascribed to A1g vibration of monoclinic Li2MnO3 (C2/m stru
• p7 scientific_body coverage=0.0: could be attributed to Eg and A1g vibrations of R-3m structure, respectively.[32,56] After 500 cycles, the A1g peak of C2/m van- ishes due to the damage to the superstructure, and the peaks of R-3m broaden and appear to redshift with a new strong peak of 625 c
• p8 scientific_body coverage=0.0: pervades the whole particle in LMRO with a thickness of 40 nm, while the Mn3+ reduction layer is remarkably limited to 6 nm in LMRO@7CuPc. Benefiting from the preservation of oxygen lat- tice framework and transition metal valence owning to CuPc re- dox strateg
• p10 scientific_body coverage=0.0: metal dissolution quantificationally. The dissolution ratios of Ni, Co, and Mn for LMRO electrode are as high as 1.177, 0.831, and 1.937 wt%, respectively, while the corresponding dissolu- tion ratios of TM elements for LMRO@7CuPcelectrode are only 0.079, 0.038
• p10 scientific_body coverage=0.062: of cationic redox reaction thus maintaining electrode capacity. The above results demonstrate that the CuPc strategy can ef- fectively restrain the decomposition of electrolytes and induce the formation of a more uniform and robust LiF-rich CEI, thus improving
• p11 back_matter coverage=0.0: Z.J.W. and C.H.Y. contributed equally to this work. The authors gratefully acknowledge the financial support from the National Key Research and Development Program of China (2022YFB2502000), the National Natural Science Foundation of China (52201277), the key p