TY - JOUR
T1 - Single Atomic Vacancy Catalysis
AU - Yang, Jieun
AU - Wang, Yan
AU - Lagos, Maureen J.
AU - Manichev, Viacheslav
AU - Fullon, Raymond
AU - Song, Xiuju
AU - Voiry, Damien
AU - Chakraborty, Sudip
AU - Zhang, Wenjing
AU - Batson, Philip E.
AU - Feldman, Leonard
AU - Gustafsson, Torgny
AU - Chhowalla, Manish
N1 - Publisher Copyright:
© 2019 American Chemical Society.
PY - 2019/9/24
Y1 - 2019/9/24
N2 - Single atom catalysts provide exceptional activity. However, measuring the intrinsic catalytic activity of a single atom in real electrochemical environments is challenging. Here, we report the activity of a single vacancy for electrocatalytically evolving hydrogen in two-dimensional (2D) MoS2. Surprisingly, we find that the catalytic activity per vacancy is not constant but increases with its concentration, reaching a sudden peak in activity at 5.7 × 1014 cm-2 where the intrinsic turn over frequency and Tafel slope of a single atomic vacancy was found to be ∼5 s-1 and 44 mV/dec, respectively. At this vacancy concentration, we also find a local strain of ∼3% and a semiconductor to metal transition in 2D MoS2. Our results suggest that, along with increasing the number of active sites, engineering the local strain and electrical conductivity of catalysts is essential in increasing their activity.
AB - Single atom catalysts provide exceptional activity. However, measuring the intrinsic catalytic activity of a single atom in real electrochemical environments is challenging. Here, we report the activity of a single vacancy for electrocatalytically evolving hydrogen in two-dimensional (2D) MoS2. Surprisingly, we find that the catalytic activity per vacancy is not constant but increases with its concentration, reaching a sudden peak in activity at 5.7 × 1014 cm-2 where the intrinsic turn over frequency and Tafel slope of a single atomic vacancy was found to be ∼5 s-1 and 44 mV/dec, respectively. At this vacancy concentration, we also find a local strain of ∼3% and a semiconductor to metal transition in 2D MoS2. Our results suggest that, along with increasing the number of active sites, engineering the local strain and electrical conductivity of catalysts is essential in increasing their activity.
KW - helium ion microscope
KW - hydrogen evolution reaction
KW - molybdenum disulfide
KW - scanning transmission electron microscope
KW - single vacancy
UR - http://www.scopus.com/inward/record.url?scp=85071653090&partnerID=8YFLogxK
U2 - 10.1021/acsnano.9b05226
DO - 10.1021/acsnano.9b05226
M3 - Article
C2 - 31398001
AN - SCOPUS:85071653090
SN - 1936-0851
VL - 13
SP - 9958
EP - 9964
JO - ACS Nano
JF - ACS Nano
IS - 9
ER -