Liquid-Phase Exfoliated GeSe Nanoflakes for Photoelectrochemical-Type Photodetectors and Photoelectrochemical Water Splitting

被引：67

作者：

Bianca, Gabriele ^{[2
,3
]}

Zappia, Marilena I. ^{[1
,4
]}

Bellani, Sebastiano ^{[1
]}

Sofer, Zdene. K. ^{[5
]}

Serri, Michele ^{[2
]}

Najafi, Leyla ^{[1
]}

Oropesa-Nunez, Reinier ^{[1
,6
]}

Martin-Garcia, Beatriz ^{[2
,7
]}

Hartman, Tomas ^{[5
]}

Leoncino, Luca ^{[8
]}

Sedmidubsky, David ^{[5
]}

Pellegrini, Vittorio ^{[1
,2
]}

Chiarello, Gennaro ^{[4
]}

Bonaccorso, Francesco ^{[1
,2
]}

机构：

[1] BeDimens Soc Azioni, I-16163 Genoa, Italy

[2] Ist Italiano Tecnol, Graphene Labs, I-16163 Genoa, Italy

[3] Univ Genoa, Dipartimento Chim & Chim Ind, I-16146 Genoa, Italy

[4] Univ Calabria, Dept Phys, I-87036 Cosenza, Italy

[5] Univ Chem & Technol Prague, Dept Inorgan Chem, Prague 16628 6, Czech Republic

[6] Uppsala Univ, Dept Mat Sci & Engn, S-75121 Uppsala, Sweden

[7] CIC NanoGUNE, Donostia San Sebastian 20018, Spain

[8] Ist Italiano Tecnol, Electron Microscopy Facil, I-16163 Genoa, Italy

来源：

ACS APPLIED MATERIALS & INTERFACES | 2020年 / 12卷 / 43期

基金：

欧盟地平线“2020”;

关键词：

germanium selenide (GeSe); photocatalysts; water splitting; two-dimensional materials; hydrogen evolution reaction (HER); oxygen evolution reaction (OER); GRAPHITIC CARBON NITRIDE; GROUP-IV MONOCHALCOGENIDES; HIGH-YIELD PRODUCTION; HYDROGEN EVOLUTION; GERMANIUM SELENIDE; SOLAR-ENERGY; ARTIFICIAL PHOTOSYNTHESIS; RAMAN-SPECTROSCOPY; OPTICAL-PROPERTIES; LAYER GRAPHENE;

D O I：

10.1021/acsami.0c14201

中图分类号：

TB3 [工程材料学];

学科分类号：

0805 ; 080502 ;

摘要：

Photoelectrochemical (PEC) systems represent powerful tools to convert electromagnetic radiation into chemical fuels and electricity. In this context, two-dimensional (2D) materials are attracting enormous interest as potential advanced photo(electro)catalysts and, recently, 2D group-IVA metal monochalcogenides have been theoretically predicted to be water splitting photocatalysts. In this work, we use density functional theory calculations to theoretically investigate the photocatalytic activity of single-/few-layer GeSe nanoflakes for both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) in pH conditions ranging from 0 to 14. Our simulations show that GeSe nanoflakes with different thickness can be mixed in the form of nanoporous films to act as nanoscale tandem systems, in which the flakes, depending on their thickness, can operate as HER- and/or OER photocatalysts. On the basis of theoretical predictions, we report the first experimental characterization of the photo(electro)catalytic activity of single-/few-layer GeSe flakes in different aqueous media, ranging from acidic to alkaline solutions: 0.5 M H2SO4 (pH 0.3), 1 M KCl (pH 6.5), and 1 M KOH (pH 14). The films of the GeSe nanoflakes are fabricated by spray coating GeSe nanoflakes dispersion in 2-propanol obtained through liquid-phase exfoliation of synthesized orthorhombic (Pnma) GeSe bulk crystals. The PEC properties of the GeSe nanoflakes are used to design PEC-type photodetectors, reaching a responsivity of up to 0.32 AW(-1) (external quantum efficiency of 86.3%) under 455 nm excitation wavelength in acidic electrolyte. The obtained performances are superior to those of several self-powered and low-voltage solution-processed photodetectors, approaching that of self-powered commercial UV-Vis photodetectors. The obtained results inspire the use of 2D GeSe in proof-of-concept water photoelectrolysis cells.

引用

页码：48598 / 48613

页数：16

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