High-Nickel Cathodes with Mechanical and Interfacial Robustness via Tailored Concentration Gradients for Stable Li-Ion Batteries

Kim, Seongwook [Pusan National Univ., Busan (Korea, Republic of)]; Thind, Arashdeep S. [Univ. of Illinois, Chicago, IL (United States)]; Mohanty, Sangram Keshari [Pusan National Univ., Busan (Korea, Republic of)] (ORCID:0000000223395733); Hong, Jeong Ki [Pusan National Univ., Busan (Korea, Republic of)]; Jung, Jae Yup [Department of Materials Science and Engineering; Kyung Hee University]; Park, Haeun [Pusan National Univ., Busan (Korea, Republic of)]; Yang, Yingjie [Univ. of Illinois, Chicago, IL (United States)] (ORCID:0000000218988171); Park, Min-Sik [Kyung Hee Univ., Seoul (Korea, Republic of)] (ORCID:0000000234902999); Porwal, Mansi Sanjay [Univ. of Illinois, Chicago, IL (United States)]; Allen, Eva [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000348506492); Choi, Byeong Kil [Pusan National Univ., Busan (Korea, Republic of)]; Jung, Hyein [Pusan National Univ., Busan (Korea, Republic of)]; Sunariwal, Neelam [Univ. of Illinois, Chicago, IL (United States)] (ORCID:0000000251158700); Kumar, Khagesh [Univ. of Illinois, Chicago, IL (United States)] (ORCID:0000000180100877); Ge, Mingyuan [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000156827443); Yoo, Jaeseung [Korea Electronics Technology Inst. (Korea, Republic of)]; Song, Jun-Ho [Korea Electronics Technology Inst. (Korea, Republic of)]; Ryu, Ji Heon [Tech Univ. of Korea (Korea, Republic of)]; Lee, Seyun [Pusan National Univ., Busan (Korea, Republic of)]; Reddy, Sri Charan [Pusan National Univ., Busan (Korea, Republic of)] (ORCID:0000000200030109); Srinivasa, Madhusudana Koratikere [Pusan National Univ., Busan (Korea, Republic of)] (ORCID:0000000169433726); Pati, Aditya Ranjan [Pusan National Univ., Busan (Korea, Republic of)]; Lee, Eungje [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000336471595); Klie, Robert F. [Univ. of Illinois, Chicago, IL (United States)] (ORCID:0000000347736667); Cabana, Jordi [Univ. of Illinois, Chicago, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000223535986); Yoo, Hyun Deog [Pusan National Univ., Busan (Korea, Republic of)] (ORCID:000000015188481X)

doi:10.1021/acsenergylett.5c01634

DOE OSTI · 2588384

High-Nickel Cathodes with Mechanical and Interfacial Robustness via Tailored Concentration Gradients for Stable Li-Ion Batteries

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Abstract

Here, we have developed a versatile mathematical framework integrated with an automated reactor system to design and reify highly customizable full concentration gradient (FCG) in high-nickel cathodes for advanced Li-ion batteries. This method provides precise and independent control of the average composition, slope, and curvature of FCGs, enabling the optimization of structural and mechanical properties of the cathode materials. We have showcased this method with Ni 0.8 Co 0.1 Mn 0.1 (OH) 2 precursors of controlled FCGs, which unlocked an optimized cathode with excellent cycling stability without crack formation after repeated cycles. This work opens up new possibilities for the design and manufacturing of advanced cathode materials, enabling safer, high-performance batteries.

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25 ENERGY STORAGE 36 MATERIALS SCIENCE batteries electrodes full concentration gradient materials precursors stability transition metals

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Kim, Seongwook [Pusan National Univ., Busan (Korea, Republic of)], Thind, Arashdeep S. [Univ. of Illinois, Chicago, IL (United States)], Mohanty, Sangram Keshari [Pusan National Univ., Busan (Korea, Republic of)] (ORCID:0000000223395733), Hong, Jeong Ki [Pusan National Univ., Busan (Korea, Republic of)], Jung, Jae Yup [Department of Materials Science and Engineering; Kyung Hee University], Park, Haeun [Pusan National Univ., Busan (Korea, Republic of)], Yang, Yingjie [Univ. of Illinois, Chicago, IL (United States)] (ORCID:0000000218988171), Park, Min-Sik [Kyung Hee Univ., Seoul (Korea, Republic of)] (ORCID:0000000234902999), Porwal, Mansi Sanjay [Univ. of Illinois, Chicago, IL (United States)], Allen, Eva [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000348506492), Choi, Byeong Kil [Pusan National Univ., Busan (Korea, Republic of)], Jung, Hyein [Pusan National Univ., Busan (Korea, Republic of)], Sunariwal, Neelam [Univ. of Illinois, Chicago, IL (United States)] (ORCID:0000000251158700), Kumar, Khagesh [Univ. of Illinois, Chicago, IL (United States)] (ORCID:0000000180100877), Ge, Mingyuan [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000156827443), Yoo, Jaeseung [Korea Electronics Technology Inst. (Korea, Republic of)], Song, Jun-Ho [Korea Electronics Technology Inst. (Korea, Republic of)], Ryu, Ji Heon [Tech Univ. of Korea (Korea, Republic of)], Lee, Seyun [Pusan National Univ., Busan (Korea, Republic of)], Reddy, Sri Charan [Pusan National Univ., Busan (Korea, Republic of)] (ORCID:0000000200030109), Srinivasa, Madhusudana Koratikere [Pusan National Univ., Busan (Korea, Republic of)] (ORCID:0000000169433726), Pati, Aditya Ranjan [Pusan National Univ., Busan (Korea, Republic of)], Lee, Eungje [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000336471595), Klie, Robert F. [Univ. of Illinois, Chicago, IL (United States)] (ORCID:0000000347736667), Cabana, Jordi [Univ. of Illinois, Chicago, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000223535986), Yoo, Hyun Deog [Pusan National Univ., Busan (Korea, Republic of)] (ORCID:000000015188481X). 2025-06-30. High-Nickel Cathodes with Mechanical and Interfacial Robustness via Tailored Concentration Gradients for Stable Li-Ion Batteries. https://doi.org/10.1021/acsenergylett.5c01634

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