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Title: Photocatalytic Overall Water Splitting at the Integrated Rh–MoRhOx Cluster Heterostructure on InGaN/GaN Nanowires

Journal Article · · Angewandte Chemie (International Edition)
ORCiD logo [1];  [2];  [1];  [1];  [1];  [3];  [1];  [1];  [4];  [1];  [2];  [1]
  1. University of Michigan, Ann Arbor, MI (United States)
  2. Cornell University, Ithaca, NY (United States)
  3. University of California, Davis, CA (United States)
  4. University of California at Davis, CA (United States)

The quest for efficient solar-driven water splitting, a promising avenue for clean fuel production, faces challenges due to limited solar energy conversion efficiency. Traditional approaches study the overall water splitting as two spatially separate half reactions on two unrelated sites, hindering full utilization of photogenerated charge and water molecules. To overcome these limitations, an integrated cluster heterostructure catalyst on InGaN/GaN semiconductor nanowires is proposed for the effective utilization of photogenerated charge carriers and water molecules on the same redox localization. By establishing the fast charge extraction kinetics based on InGaN/GaN nanowires, the integration of Rh and MoRhOx clusters on the nanowire surface enables simultaneous and fast hydrogen/oxygen evolution reactions at the cluster heterostructure. Furthermore, the integrated strategy can enhance the charge redistribution across the heterostructure between the two clusters, further optimizing adsorption of reaction intermediates on each cluster for boosted photocatalytic water splitting activity. Consequently, the integrated heterostructure triggers a 40-fold increased hydrogen production efficiency in an artificial leaf system. This study provides valuable insights for the rational design of advanced heterostructured photocatalysts for water splitting and beyond.

Research Organization:
Cornell Univ., Ithaca, NY (United States); Univ. of California, Davis, CA (United States); Univ. of Michigan, Ann Arbor, MI (United States); University of California, Davis, CA (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); United States Army Research Office
Grant/Contract Number:
SC0004911; SC0015329
OSTI ID:
3005197
Journal Information:
Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 2 Vol. 65; ISSN 1521-3773; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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