Artificial Photosynthesis with Polymeric Carbon Nitride: When Meeting Metal Nanoparticles, Single Atoms, and Molecular Complexes

Li, Yanrui; Kong, Tingting; Shen, Shaohua

doi:10.1002/smll.201900772

Cited by 102 publications

(63 citation statements)

References 153 publications

(241 reference statements)

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“…Large numbers of active sites in metal molecular complexes allow the complexes to intimately interact with PCN to capture photoexcited electrons from PCN. [24][25][26][27][28] However, these metal molecular complexes usually possess weak electron-capturing capabilities. Most importantly, all these PHE reactions over above mentioned PHJ and MHJ photocatalysts were conducted under vacuum conditions.…”

Section: Introductionmentioning

confidence: 99%

Photocatalytic Hydrogen Evolution under Ambient Conditions on Polymeric Carbon Nitride/Donor‐π‐Acceptor Organic Molecule Heterostructures

Wang

Chen

et al. 2020

Adv Funct Materials

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Efficient solar-to-hydrogen (STH) energy conversion under ambient conditions (room temperature and atmospheric pressure) is important for pursuing scalable solar hydrogen generation. Modification of polymeric carbon nitride (PCN) by conjugated polymers has attracted great attention for improving photocatalytic hydrogen evolution (PHE) performance. However, the limited interfacial junction between PCN and conjugated polymers leads to a low density of free charges, resulting in unsatisfactory PHE activity. Herein, three donor-π-acceptor-structured organic molecules (OMs) with different electron-donating units (amino, N,N-diethyl and triphenylamine) and same electron-accepting unit (benzothiadiazole) are designed to modify PCN to enlarge the interfacial junction. The optimized PHE performance under AM 1.5G simulated sunlight and ambient conditions can maintain as high as 4.63 mmol h −1 g −1 (the highest record among all the reported PCN-based photocatalysts to the best of the authors knowledge). The improved performance can be partially attributed to the strong visible light harvesting capability of OMs. Specifically, the triphenylamine unit in the formed type II molecule heterojunctions (MHJ) enables efficient charge separation at the interfacial junction, which prolongs the photogenerated electron lifetime for PHE. The designed MHJ photocatalysts show outstanding PHE performance under ambient conditions, which is highly promising for scalable STH conversion.

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Section: Introductionmentioning

confidence: 99%

Photocatalytic Hydrogen Evolution under Ambient Conditions on Polymeric Carbon Nitride/Donor‐π‐Acceptor Organic Molecule Heterostructures

Wang

Chen

et al. 2020

Adv Funct Materials

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“…Furthermore, different types of photosensitizers could have diverse advantages. The combining of above-mentioned systems could significantly improve the performance of constructed hybrid nanostructures [63][64][65][66][67]. Integration and application of the photo-enzyme-coupled catalytic system (Figs.…”

Section: Construction Of Photo-enzyme-coupled Catalytic Systemmentioning

confidence: 99%

Advances in photo-enzymatic-coupling catalysis system

Bai

Wang

2021

Syst Microbiol and Biomanuf

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Photosynthesis, as an efficient pathway for solar energy capture and utilization, has supported aerobionts for billions of years. The imitation of photosynthesis to construct artificial photo-enzymatic-coupling catalysis system has become a powerful means to solve energy and environmental problems. After years of in-depth research on this coupled system, through ingenious and rational design, the synergistic effect of photo-and enzymatic catalyses has played a significant role in many different fields, including solar-driven fuel production, chiral chemical synthesis and carbon dioxide fixation. Furthermore, light in enzymatic catalysis could also endow enzyme new possibilities. Photo-induced radical cofactor could bring catalytic promiscuity to enzymes, making them catalyze reactions that natural enzymes cannot. This review summarizes the advances in photo-enzymatic-coupling catalysis system and introduces its essential components, their integration and application. The possibilities presented by photo-induced catalytic promiscuity and its significance for expanding the toolbox of enzymes are also discussed.

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“…Metal nanoparticle/semiconductor hybrids with various morphologies and sizes have been widely used in photocatalysis. [ 196,197 ] Ye and co‐workers reported the direct growth of noble metal (e.g., Pt, Au, Rh, and Ag) particles on defective WO 3 nanorods. [ 194 ] The authors observed that the oxidative metal ions and WO 2.72 nanostructures with V O ‐induced reducibility were immediately nucleated at V O sites, growing into noble metal clusters and nanoparticles.…”

Section: Defect‐induced Heterostructurementioning

confidence: 99%

Atomic‐Level and Modulated Interfaces of Photocatalyst Heterostructure Constructed by External Defect‐Induced Strategy: A Critical Review

Zhang

et al. 2020

Small

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Despite the existence of numerous photocatalyst heterostructures, their separation efficiency and charge flow precision remain low due to the poor study on interfacial properties. The photocatalysts with confined defects can effectively control the photogenerated carrier migration, but the metastability of such defects considerably decreases the photocatalyst stability. Meanwhile, the introduction of defective region can increase the coordinative unsaturation and delocalize local electrons to promote their interactions with the molecules/ions in that region. The selective growth of modulated heterogeneous interface by defect‐induced strategy may not only increase the stability of defective structures, but also enhance the migration of interfacial charges. Using this method, photocatalytic heterostructures with low contact resistances and intimate interfaces are constructed to achieve the optimal charge migration in terms of efficiency and accuracy. In this work, the point, linear, and planar heterogeneous interfaces and related defect engineering techniques are discussed. Particularly, it is focused on the external, defect‐induced interfacial heterogeneities with various spatial and dimensional configurations, which exhibit modulated and controllable interfacial properties. Furthermore, the main aspects of fabricating photocatalyst heterostructures by the defect‐induced strategy, including the i) controllable generation of defects, ii) advanced characterization methods, and iii) elaborate construction of the minimal interface, are described.

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Artificial Photosynthesis with Polymeric Carbon Nitride: When Meeting Metal Nanoparticles, Single Atoms, and Molecular Complexes

Cited by 102 publications

References 153 publications

Photocatalytic Hydrogen Evolution under Ambient Conditions on Polymeric Carbon Nitride/Donor‐π‐Acceptor Organic Molecule Heterostructures

Photocatalytic Hydrogen Evolution under Ambient Conditions on Polymeric Carbon Nitride/Donor‐π‐Acceptor Organic Molecule Heterostructures

Advances in photo-enzymatic-coupling catalysis system

Atomic‐Level and Modulated Interfaces of Photocatalyst Heterostructure Constructed by External Defect‐Induced Strategy: A Critical Review

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