Title: Hybrid 0D–2D black phosphorus quantum dots–graphitic carbon nitride nanosheets for efficient hydrogen evolution

Abstract

As an emerging post-graphene two-dimensional (2D) nanomaterial, black phosphorus (BP) is attracting a great deal of current attention for the direct conversion of solar energy into solar fuels on account of its unique tunable direct-bandgap and high charge-carrier mobility. Herein, for the first time, we immobilize BP quantum dots (BPQDs) onto graphitic carbon nitride (g-C₃N₄) nanosheets to create a 0D-2D inorganic-organic hybrid via a conventional and cost–effective sonication approach. The as-prepared BPQDs/g-C₃N₄ hybrids display BPQD content-dependent performance in visible-light-driven hydrogen generation. 5 wt% BPQDs/g-C₃N₄ with cyclability exhibits the greatest hydrogen evolution rate of 271 μmol h-1 g-1 that is 5.6 and 4.2 times greater than that of pristine g-C₃N₄ and BPQDs, respectively. We demonstrate that the type-II band alignment, the formation of phosphorus–carbon bonds and the efficient interfacial charge separation between well-dispersed BPQDs and g-C₃N₄ synergetically enhance the photoactivity and photostability. In conclusion, this study opens possibilities to create viable BP-based heterostructures for energy conversion and storage.

Authors:

Lei, Wanying ^[1]; Mi, Yang ^[2]; Feng, Rongjuan ^[2]; Liu, Ping  ^[3];

• Search DOE PAGES for author "Liu, Ping"
• Search DOE PAGES for ORCID "0000-0001-8363-070X"

Hu, Song ^[2]; Yu, Jiaguo  ^[4];

• Search DOE PAGES for author "Yu, Jiaguo"
• Search DOE PAGES for ORCID "0000-0002-0612-8633"

Liu, Xinfeng ^[2]; Rodriguez, José A.  ^[3];

• Search DOE PAGES for author "Rodriguez, José A."
• Search DOE PAGES for ORCID "0000-0002-5680-4214"

Wang, Jia-ou ^[5]; Zheng, Lei ^[5]; Tang, Kun ^[5]; Zhu, Sixu ^[5]; Liu, Gang ^[2]; Liu, Minghua ^[6]

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+ Show Author Affiliations

1. National Center for Nanoscience and Technology, Beijing (China). CAS Key Lab. of Standardization and Measurement for Nanotechnology, CAS Center for Excellence in Nanoscience; Peking Univ., Beijing (China). Academy for Advanced Interdisciplinary Studies; Univ. of Chinese Academy of Sciences, Beijing (China)
2. National Center for Nanoscience and Technology, Beijing (China). CAS Key Lab. of Standardization and Measurement for Nanotechnology, CAS Center for Excellence in Nanoscience
3. Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry
4. Wuhan Univ. of Technology (China). State Key Lab. of Advanced Technology for Materials Synthesis and Processing
5. Chinese Academy of Sciences (CAS), Beijing (China). Beijing Synchrotron Radiation Facility, Inst. of High Energy Physics
6. National Center for Nanoscience and Technology, Beijing (China). CAS Key Lab. of Standardization and Measurement for Nanotechnology, CAS Center for Excellence in Nanoscience; Univ. of Chinese Academy of Sciences, Beijing (China)

Publication Date:

Wed Aug 01 00:00:00 EDT 2018

Research Org.:

Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1466590

Alternate Identifier(s):

OSTI ID: 1608353

Report Number(s):

BNL-207995-2018-JAAM
Journal ID: ISSN 2211-2855

Grant/Contract Number:  

SC0012704; AC02-05CH11231

Resource Type:

Accepted Manuscript

Journal Name:

Nano Energy

Additional Journal Information:

Journal Volume: 50; Journal Issue: C; Journal ID: ISSN 2211-2855

Publisher:

Elsevier

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE