Synergistic Ru Species on Poly(heptazine imide) Enabling Efficient Photocatalytic CO2 Reduction with H2O beyond 800 nm - Details

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Photocatalytic　CO2　conversion　with　H2O　to　carbonaceous　fuels　is　a　desirable　strategy　for　CO2　management　and　solar　utilization,　yet　its　efficiency　remains　suboptimal.　Herein,　efficient　and　durable　CO2　photoreduction　is　realized　over　a　RuNPs/Ru-PHI　catalyst　assembled　by　anchoring　Ru　single　atoms　(SAs)　and　nanoparticles　(NPs)　onto　poly(heptazine　imide)　(PHI)　via　the　in-plane　Ru-N4　coordination　and　interfacial　Ru-N　bonds,　respectively.　This　catalyst　shows　an　unsurpassed　CO　production　(32.8 µmol　h−1),　a　record-high　apparent　quantum　efficiency　(0.26%)　beyond　800 nm,　and　the　formation　of　the　valuable　H2O2.　Ru　SAs　tune　PHI＇s　electronic　structure　to　promote　in-plane　charge　transfer　to　Ru　NPs,　forming　a　built-in　electron　field　at　the　interface,　which　directs　electron-hole　separation　and　rushes　excited　electron　movement　from　Ru-PHI　to　Ru　NPs.　Simultaneously,　Ru　SAs　introduce　an　impurity　level　in　PHI　to　endow　long-wavelength　photoabsorption,　while　Ru　NPs　strengthen　CO2　adsorption/activation　and　expedite　CO　desorption.　These　effects　of　Ru　species　together　effectively　ensure　CO2-to-CO　conversion.　The　CO2　reduction　on　the　catalyst　is　revealed　to　follow　the　pathway　CO2→　*CO2→　*COOH→　*CO→　CO,　based　on　the　intermediates　identified　by　in　situ　diffuse　reflectance　infrared　Fourier　transform　spectroscopy　and　further　supported　by　density　functional　theory　calculations.　©　2025　Wiley-VCH　GmbH.

Keyword：

Carbon nitrides CO2 reduction Photocatalysis Poly (heptazine imide)

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[ 1 ] [Su B.]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 2 ] [Su B.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 3 ] [Wang S.]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 4 ] [Wang S.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 5 ] [Xing W.]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 6 ] [Xing W.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 7 ] [Liu K.]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 8 ] [Liu K.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 9 ] [Hung S.-F.]Department of Applied Chemistry and Center for Emergent Functional Matter Science, National Yang Ming Chiao Tung University, Hsinchu, 300, Taiwan
[ 10 ] [Chen X.]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 11 ] [Chen X.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 12 ] [Fang Y.]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 13 ] [Fang Y.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 14 ] [Zhang G.]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 15 ] [Zhang G.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 16 ] [Zhang H.]KAUST Catalysis Center, Physical Sciences and Engineering Division, King Abdullah University of Science and Technology, Thuwal, 23955, Saudi Arabia
[ 17 ] [Wang X.]State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 18 ] [Wang X.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China

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Angewandte Chemie - International Edition

ISSN： 1433-7851

Year： 2025

1 6 . 1 0 0

JCR@2023

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