Molecular co-catalyst accelerating hole transfer for enhanced photocatalytic H2 evolution.
In artificial photocatalysis, sluggish kinetics of hole transfer and the resulting high-charge recombination rate have been the Achilles' heel of photocatalytic conversion efficiency. Here we demonstrate water-soluble molecules as co-catalysts to accelerate hole transfer for improved photocatalytic H2 evolution activity. Trifluoroacetic acid (TFA), by virtue of its reversible redox couple TFA·/TFA(-), serves as a homogeneous co-catalyst that not only maximizes the contact areas between co-catalysts and reactants but also greatly promotes hole transfer. Thus K4Nb6O17 nanosheet catalysts achieve drastically increased photocatalytic H2 production rate in the presence of TFA, up to 32 times with respect to the blank experiment. The molecular co-catalyst represents a new, simple and highly effective approach to suppress recombination of photogenerated charges, and has provided fertile new ground for creating high-efficiency photosynthesis systems, avoiding use of noble-metal co-catalysts.
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, Synergetic Innovation Center of Quantum Information and Quantum Physics, Hefei Science Center of CAS, CAS Key Laboratory of Mechanical Behavior and Design of Materials, University of Science and Technology of China, Hefei 230026, Anhui, China.
Wentuan
W
Bi
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, Synergetic Innovation Center of Quantum Information and Quantum Physics, Hefei Science Center of CAS, CAS Key Laboratory of Mechanical Behavior and Design of Materials, University of Science and Technology of China, Hefei 230026, Anhui, China.
Xiaogang
X
Li
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, Synergetic Innovation Center of Quantum Information and Quantum Physics, Hefei Science Center of CAS, CAS Key Laboratory of Mechanical Behavior and Design of Materials, University of Science and Technology of China, Hefei 230026, Anhui, China.
Lei
L
Zhang
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, Synergetic Innovation Center of Quantum Information and Quantum Physics, Hefei Science Center of CAS, CAS Key Laboratory of Mechanical Behavior and Design of Materials, University of Science and Technology of China, Hefei 230026, Anhui, China.
Tao
T
Jin
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230026, Anhui, China.
Lidong
L
Zhang
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, Synergetic Innovation Center of Quantum Information and Quantum Physics, Hefei Science Center of CAS, CAS Key Laboratory of Mechanical Behavior and Design of Materials, University of Science and Technology of China, Hefei 230026, Anhui, China.
Qun
Q
Zhang
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, Synergetic Innovation Center of Quantum Information and Quantum Physics, Hefei Science Center of CAS, CAS Key Laboratory of Mechanical Behavior and Design of Materials, University of Science and Technology of China, Hefei 230026, Anhui, China.
Yi
Y
Luo
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, Synergetic Innovation Center of Quantum Information and Quantum Physics, Hefei Science Center of CAS, CAS Key Laboratory of Mechanical Behavior and Design of Materials, University of Science and Technology of China, Hefei 230026, Anhui, China.
Changzheng
C
Wu
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, Synergetic Innovation Center of Quantum Information and Quantum Physics, Hefei Science Center of CAS, CAS Key Laboratory of Mechanical Behavior and Design of Materials, University of Science and Technology of China, Hefei 230026, Anhui, China.
Yi
Y
Xie