Monolayered g-C3N4 nanosheet as an emerging cationic building block for bifunctional 2D superlattice hybrid catalysts with controlled defect structures

Nam Hee Kwon; Seung Jae Shin; Xiaoyan Jin; Youngae Jung; Geum Sook Hwang; Hyungjun Kim; Seong Ju Hwang

doi:10.1016/j.apcatb.2020.119191

Monolayered g-C₃N₄ nanosheet as an emerging cationic building block for bifunctional 2D superlattice hybrid catalysts with controlled defect structures

Nam Hee Kwon, Seung Jae Shin, Xiaoyan Jin, Youngae Jung, Geum Sook Hwang, Hyungjun Kim, Seong Ju Hwang

Department of Materials Science and Engineering

Research output: Contribution to journal › Article › peer-review

42 Citations (Scopus)

Abstract

New class of superlattice nanohybrids of interstratified graphitic-carbon nitride (g-C₃N₄)–transition metal dichalcogenide monolayers are synthesized by employing pH-controlled g-C₃N₄ nanosheet (NS) as an emerging cationic building block. The interstratification of g-C₃N₄ and MoS₂ NSs leads to strong interfacial electronic coupling, creation of nitrogen vacancy, and stabilization of 1T′-MoS₂ phase. The superlattice g-C₃N₄–MoS₂ nanohybrids display remarkably enhanced bifunctionality as photocatalysts for visible light-induced N₂ fixation and electrocatalysts for hydrogen evolution. Of prime importance is that the creation of nitrogen vacancy results in the significant improvement of selectivity for photocatalytic N₂ fixation (582 μmolL⁻¹h⁻¹) over competitive photocatalytic H₂ generation. This is attributable to promoted adsorption of nitrogen, provision of many active sites, and enhancement of charge transfer kinetics, charge separation, and visible light absorptivity. This study highlights that the application of g-C₃N₄ NS as a cationic building block provides valuable opportunity to widen the library of multifunctional NS-based superlattice nanohybrids.

Original language	English
Article number	119191
Journal	Applied Catalysis B: Environmental
Volume	277
DOIs	https://doi.org/10.1016/j.apcatb.2020.119191
Publication status	Published - 2020 Nov 15

Bibliographical note

Funding Information:
This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIP) (No. NRF-2017R1A2A1A17069463 ), by the Korea government (MSIT) (No. NRF-2017R1A5A1015365 ), and by the Korea government (MSIP) (No. NRF-2020R1A2C3008671 ). The experiments at PAL were supported in part by MOST and POSTECH.

Publisher Copyright:
© 2020 Elsevier B.V.

All Science Journal Classification (ASJC) codes

Catalysis
Environmental Science(all)
Process Chemistry and Technology

Access to Document

10.1016/j.apcatb.2020.119191

Cite this

@article{f578b9e8d3664fac85b4811cedc9d8f0,

title = "Monolayered g-C3N4 nanosheet as an emerging cationic building block for bifunctional 2D superlattice hybrid catalysts with controlled defect structures",

abstract = "New class of superlattice nanohybrids of interstratified graphitic-carbon nitride (g-C3N4)–transition metal dichalcogenide monolayers are synthesized by employing pH-controlled g-C3N4 nanosheet (NS) as an emerging cationic building block. The interstratification of g-C3N4 and MoS2 NSs leads to strong interfacial electronic coupling, creation of nitrogen vacancy, and stabilization of 1T′-MoS2 phase. The superlattice g-C3N4–MoS2 nanohybrids display remarkably enhanced bifunctionality as photocatalysts for visible light-induced N2 fixation and electrocatalysts for hydrogen evolution. Of prime importance is that the creation of nitrogen vacancy results in the significant improvement of selectivity for photocatalytic N2 fixation (582 μmolL−1h−1) over competitive photocatalytic H2 generation. This is attributable to promoted adsorption of nitrogen, provision of many active sites, and enhancement of charge transfer kinetics, charge separation, and visible light absorptivity. This study highlights that the application of g-C3N4 NS as a cationic building block provides valuable opportunity to widen the library of multifunctional NS-based superlattice nanohybrids.",

author = "Kwon, {Nam Hee} and Shin, {Seung Jae} and Xiaoyan Jin and Youngae Jung and Hwang, {Geum Sook} and Hyungjun Kim and Hwang, {Seong Ju}",

note = "Funding Information: This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIP) (No. NRF-2017R1A2A1A17069463 ), by the Korea government (MSIT) (No. NRF-2017R1A5A1015365 ), and by the Korea government (MSIP) (No. NRF-2020R1A2C3008671 ). The experiments at PAL were supported in part by MOST and POSTECH. Publisher Copyright: {\textcopyright} 2020 Elsevier B.V.",

year = "2020",

month = nov,

day = "15",

doi = "10.1016/j.apcatb.2020.119191",

language = "English",

volume = "277",

journal = "Applied Catalysis B: Environmental",

issn = "0926-3373",

publisher = "Elsevier",

}

TY - JOUR

T1 - Monolayered g-C3N4 nanosheet as an emerging cationic building block for bifunctional 2D superlattice hybrid catalysts with controlled defect structures

AU - Kwon, Nam Hee

AU - Shin, Seung Jae

AU - Jin, Xiaoyan

AU - Jung, Youngae

AU - Hwang, Geum Sook

AU - Kim, Hyungjun

AU - Hwang, Seong Ju

N1 - Funding Information: This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIP) (No. NRF-2017R1A2A1A17069463 ), by the Korea government (MSIT) (No. NRF-2017R1A5A1015365 ), and by the Korea government (MSIP) (No. NRF-2020R1A2C3008671 ). The experiments at PAL were supported in part by MOST and POSTECH. Publisher Copyright: © 2020 Elsevier B.V.

PY - 2020/11/15

Y1 - 2020/11/15

N2 - New class of superlattice nanohybrids of interstratified graphitic-carbon nitride (g-C3N4)–transition metal dichalcogenide monolayers are synthesized by employing pH-controlled g-C3N4 nanosheet (NS) as an emerging cationic building block. The interstratification of g-C3N4 and MoS2 NSs leads to strong interfacial electronic coupling, creation of nitrogen vacancy, and stabilization of 1T′-MoS2 phase. The superlattice g-C3N4–MoS2 nanohybrids display remarkably enhanced bifunctionality as photocatalysts for visible light-induced N2 fixation and electrocatalysts for hydrogen evolution. Of prime importance is that the creation of nitrogen vacancy results in the significant improvement of selectivity for photocatalytic N2 fixation (582 μmolL−1h−1) over competitive photocatalytic H2 generation. This is attributable to promoted adsorption of nitrogen, provision of many active sites, and enhancement of charge transfer kinetics, charge separation, and visible light absorptivity. This study highlights that the application of g-C3N4 NS as a cationic building block provides valuable opportunity to widen the library of multifunctional NS-based superlattice nanohybrids.

AB - New class of superlattice nanohybrids of interstratified graphitic-carbon nitride (g-C3N4)–transition metal dichalcogenide monolayers are synthesized by employing pH-controlled g-C3N4 nanosheet (NS) as an emerging cationic building block. The interstratification of g-C3N4 and MoS2 NSs leads to strong interfacial electronic coupling, creation of nitrogen vacancy, and stabilization of 1T′-MoS2 phase. The superlattice g-C3N4–MoS2 nanohybrids display remarkably enhanced bifunctionality as photocatalysts for visible light-induced N2 fixation and electrocatalysts for hydrogen evolution. Of prime importance is that the creation of nitrogen vacancy results in the significant improvement of selectivity for photocatalytic N2 fixation (582 μmolL−1h−1) over competitive photocatalytic H2 generation. This is attributable to promoted adsorption of nitrogen, provision of many active sites, and enhancement of charge transfer kinetics, charge separation, and visible light absorptivity. This study highlights that the application of g-C3N4 NS as a cationic building block provides valuable opportunity to widen the library of multifunctional NS-based superlattice nanohybrids.

UR - http://www.scopus.com/inward/record.url?scp=85085925399&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85085925399&partnerID=8YFLogxK

U2 - 10.1016/j.apcatb.2020.119191

DO - 10.1016/j.apcatb.2020.119191

M3 - Article

AN - SCOPUS:85085925399

SN - 0926-3373

VL - 277

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

M1 - 119191

ER -