TY - JOUR
T1 - Interfacial Modification of Lithium Metal Anode by Boron Nitride Nanosheets
AU - Wang, Zhiyu
AU - Qin, Si
AU - Chen, Fangfang
AU - Chen, Shasha
AU - Liu, Dan
AU - Jiang, Degang
AU - Zhang, Peng
AU - Mota-Santiago, Pablo
AU - Hegh, Dylan
AU - Lynch, Peter
AU - Alotabi, Abdulrahman S.
AU - Andersson, Gunther G.
AU - Howlett, Patrick C.
AU - Forsyth, Maria
AU - Lei, Weiwei
AU - Razal, Joselito M.
PY - 2024/1/30
Y1 - 2024/1/30
N2 - Metallic lithium (Li) is the most attractive anode for Li batteries because it holds the highest theoretical specific capacity (3860 mA h g-1) and the lowest redox potential (−3.040 V vs SHE). However, the poor interface stability of the Li anode, which is caused by the high reactivity and dendrite formation of metallic Li upon cycling, leads to undesired electrochemical performance and safety issues. While two-dimensional boron nitride (BN) nanosheets have been utilized as an interfacial layer, the mechanism on how they stabilize the Li-electrolyte interface remains elusive. Here, we show how BN nanosheet interlayers suppress Li dendrite formation, enhance Li ion transport kinetics, facilitate Li deposition, and reduce electrolyte decomposition. We show through both simulation and experimental data that the desolvation process of a solvated Li ion within the interlayer nanochannels kinetically favors Li deposition. This process enables long cycling stability, reduced voltage polarization, improved interface stability, and negligible volume expansion. Their application as an interfacial layer in symmetric cells and full cells that display significantly improved electrochemical properties is also demonstrated. The knowledge gained in this study provides both critical insights and practical guidelines for designing a Li metal anode with significantly improved performance.
AB - Metallic lithium (Li) is the most attractive anode for Li batteries because it holds the highest theoretical specific capacity (3860 mA h g-1) and the lowest redox potential (−3.040 V vs SHE). However, the poor interface stability of the Li anode, which is caused by the high reactivity and dendrite formation of metallic Li upon cycling, leads to undesired electrochemical performance and safety issues. While two-dimensional boron nitride (BN) nanosheets have been utilized as an interfacial layer, the mechanism on how they stabilize the Li-electrolyte interface remains elusive. Here, we show how BN nanosheet interlayers suppress Li dendrite formation, enhance Li ion transport kinetics, facilitate Li deposition, and reduce electrolyte decomposition. We show through both simulation and experimental data that the desolvation process of a solvated Li ion within the interlayer nanochannels kinetically favors Li deposition. This process enables long cycling stability, reduced voltage polarization, improved interface stability, and negligible volume expansion. Their application as an interfacial layer in symmetric cells and full cells that display significantly improved electrochemical properties is also demonstrated. The knowledge gained in this study provides both critical insights and practical guidelines for designing a Li metal anode with significantly improved performance.
KW - boron nitride
KW - dendrite suppression
KW - desolvation
KW - lithium metal anodes
KW - two-dimensional nanomaterials
UR - http://www.scopus.com/inward/record.url?scp=85183523825&partnerID=8YFLogxK
UR - http://purl.org/au-research/grants/ARC/CE140100012
UR - http://purl.org/au-research/grants/ARC/DP190103290
UR - http://purl.org/au-research/grants/ARC/DP220103416
UR - http://purl.org/au-research/grants/ARC/FT200100730
UR - http://purl.org/au-research/grants/ARC/FT210100804
U2 - 10.1021/acsnano.3c11135
DO - 10.1021/acsnano.3c11135
M3 - Article
C2 - 38236027
AN - SCOPUS:85183523825
SN - 1936-0851
VL - 18
SP - 3531
EP - 3541
JO - ACS nano
JF - ACS nano
IS - 4
ER -