TY - JOUR
T1 - Black Ultrathin Single-Crystalline Flakes of CuVP2S6 and CuCrP2S6 for Near-Infrared-Driven Photocatalytic Hydrogen Evolution
AU - Lin, Bo
AU - Duan, Ruihuan
AU - Li, Yonghui
AU - Hua, Weibo
AU - Zhou, Yao
AU - Zhou, Jiadong
AU - Di, Jun
AU - Luo, Xiao
AU - Li, He
AU - Zhao, Wenting
AU - Yang, Guidong
AU - Liu, Zheng
AU - Liu, Fucai
N1 - Publisher Copyright:
© 2024 Wiley-VCH GmbH.
PY - 2024/8/8
Y1 - 2024/8/8
N2 - The development of new near-infrared-responsive photocatalysts is a fascinating and challenging approach to acquire high photocatalytic hydrogen evolution (PHE) performance. Herein, near-infrared-responsive black CuVP2S6 and CuCrP2S6 flakes, as well as CuInP2S6 flakes, are designed and constructed for PHE. Atom-resolved scanning transmission electron microscopy images and X-ray absorption fine structure evidence the formation of ultrathin single-crystalline sheet-like structure of CuVP2S6 and CuCrP2S6. The synthetic CuVP2S6 and CuCrP2S6, with a narrow bandgap of ≈1.0 eV, shows the high light-absorption edge exceeding 1100 nm. Moreover, through the femtosecond-resolved transient absorption spectroscopy, CuCrP2S6 displays the efficient charge transfer and long charge lifetime (18318.1 ps), which is nearly 3 and 29 times longer than that of CuVP2S6 and CuInP2S6, respectively. In addition, CuCrP2S6, with the appropriate d-band and p-band, is thermodynamically favorable for the H+ adsorption and H2 desorption by contrast with CuVP2S6 and CuInP2S6. As a result, CuCrP2S6 exhibits high PHE rates of 9.12 and 0.66 mmol h−1 g−1 under simulated sunlight and near-infrared light irradiation, respectively, far exceeding other layered metal phospho–sulfides. This work offers a distinctive perspective for the development of new near-infrared-responsive photocatalysts.
AB - The development of new near-infrared-responsive photocatalysts is a fascinating and challenging approach to acquire high photocatalytic hydrogen evolution (PHE) performance. Herein, near-infrared-responsive black CuVP2S6 and CuCrP2S6 flakes, as well as CuInP2S6 flakes, are designed and constructed for PHE. Atom-resolved scanning transmission electron microscopy images and X-ray absorption fine structure evidence the formation of ultrathin single-crystalline sheet-like structure of CuVP2S6 and CuCrP2S6. The synthetic CuVP2S6 and CuCrP2S6, with a narrow bandgap of ≈1.0 eV, shows the high light-absorption edge exceeding 1100 nm. Moreover, through the femtosecond-resolved transient absorption spectroscopy, CuCrP2S6 displays the efficient charge transfer and long charge lifetime (18318.1 ps), which is nearly 3 and 29 times longer than that of CuVP2S6 and CuInP2S6, respectively. In addition, CuCrP2S6, with the appropriate d-band and p-band, is thermodynamically favorable for the H+ adsorption and H2 desorption by contrast with CuVP2S6 and CuInP2S6. As a result, CuCrP2S6 exhibits high PHE rates of 9.12 and 0.66 mmol h−1 g−1 under simulated sunlight and near-infrared light irradiation, respectively, far exceeding other layered metal phospho–sulfides. This work offers a distinctive perspective for the development of new near-infrared-responsive photocatalysts.
KW - black ultrathin CuCrPS flakes
KW - black ultrathin CuVPS flakes
KW - layered metal phospho–sulfides
KW - narrow bandgap
KW - near-infrared-responsive photocatalysts
UR - http://www.scopus.com/inward/record.url?scp=85196030584&partnerID=8YFLogxK
U2 - 10.1002/adma.202404833
DO - 10.1002/adma.202404833
M3 - Article
AN - SCOPUS:85196030584
SN - 0935-9648
VL - 36
JO - Advanced Materials
JF - Advanced Materials
IS - 32
M1 - 2404833
ER -