Organic Photovoltaic Catalyst with Extended Exciton Diffusion for High-Performance Solar Hydrogen Evolution

Zhu, Yuying; Zhang, Zhenzhen; Si, Wenqin; Sun, Qianlu; Cai, Guilong; Li, Yawen; Jia, Yixiao; Lu, Xinhui; Xu, Weigao; Zhang, Shiming; Lin, Yuze

doi:10.1021/jacs.2c03161

Cited by 46 publications

(52 citation statements)

References 68 publications

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“…Compared with PCCP , the much smaller radius of PBNP (Figure c) is beneficial to charge transfer. These results are consistent with those of the built-in electric field, further supporting the performance that the B–N bond alters the electronic structure of the polymer and is beneficial for promoting photocatalytic water splitting. , …”

Section: Resultssupporting

confidence: 80%

“…The exciton binding energy E b is the Coulomb potential between the photo-generated electrons/holes and reflects the separation of photo-generated electrons/holes, which represents the ability of the photo-generated electrons/holes to separate and diffuse efficiently into the reaction interface. − To compare the effects on the conjugated polymers PCCP and PBNP , the E b can be approximated by combining the Arrhenius equation I ( T ) = I 0 /( 1 + A exp(− E b / k B T ) and the temperature-dependent PL spectroscopies (Figure S12). The experimental results show that the E b of PCCP is 85 meV and that of PBNP is 53 meV (Figure d), indicating that the substitution of the B–N bond can effectively reduce the E b of the samples.…”

Section: Resultsmentioning

confidence: 99%

“…These results are consistent with those of the built-in electric field, further supporting the performance that the B−N bond alters the electronic structure of the polymer and is beneficial for promoting photocatalytic water splitting. 42,47 The exciton binding energy E b is the Coulomb potential between the photo-generated electrons/holes and reflects the separation of photo-generated electrons/holes, which represents the ability of the photo-generated electrons/holes to separate and diffuse efficiently into the reaction interface. 47−49 To compare the effects on the conjugated polymers PCCP and PBNP, the E b can be approximated by combining the Arrhenius equation I(T) = I 0 /(1 + A exp(−E b /k B T) and the temperature-dependent PL spectroscopies (Figure S12).…”

Section: ■ Results and Discussionmentioning

confidence: 99%

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Construction of Efficient D–A-Type Photocatalysts by B–N Bond Substitution for Water Splitting

Chen

et al. 2023

Macromolecules

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Donor−acceptor (D−A)-type conjugated polymers are emerging as a promising platform for solar to chemical energy conversion, such as water splitting to H 2 production. Disclosed herein is a new strategy that makes it possible to transform conventional conjugated polymers into D−A-type conjugated polymers by B−N bond substitution while retaining the original backbone. Using this method, we synthesize two conjugated polymers PCCP and PBNP, where PBNP containing the B−N bonds has a strong built-in electric field and a lower exciton binding energy (E b ) for solar-driven photocatalytic hydrogen evolution. PBNP without any co-catalyst addition exhibits a high hydrogen evolution rate (HER) of more than 9445 μmol g −1 h −1 for water splitting under AM 1.5G sunlight illumination (100 mW cm −2 ), a 28 times improvement relative to PCCP (333 μmol g −1 h −1 ). In addition, another contrasting BN-substituted D−A polymer PBNN also exhibits an excellent HER of 5740 μmol g −1 h −1 . Theoretical and experimental studies confirm that the substitution of B−N bonds can completely change the electronic properties of the original polymer, allowing rapid charge separation and transfer. This work opens up new prospects for the preparation of efficient D−A conjugated polymer photocatalysts.

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Section: Resultssupporting

confidence: 80%

Section: Resultsmentioning

confidence: 99%

Section: ■ Results and Discussionmentioning

confidence: 99%

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Construction of Efficient D–A-Type Photocatalysts by B–N Bond Substitution for Water Splitting

Chen

et al. 2023

Macromolecules

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“…Encouraged by solar energy to electricity conversion efficiency of 18–20 % achieved in organic photovoltaic cells, [14] organic photovoltaic materials with broad absorption, have attracted increasing attention in photocatalytic hydrogen production as homogeneous or heterogeneous catalysts, and then greatly enhanced photocatalytic hydrogen evolution rate (HER), [6a,g, 15] relative to traditional inorganic photocatalysts, such as TiO 2 , [3b] CdS [16] . McCulloch and co‐workers exhibited that organic photovoltaic heterojunction nanoparticles (NPs) could obtain much higher HER than those of their corresponding single‐component NPs, [6c,d] while Cooper and co‐workers realized high HER by employing polymer/fullerene heterojunction [6d] .…”

Section: Introductionmentioning

confidence: 99%

Organic Photovoltaic Catalyst with σ‐π Anchor for High‐Performance Solar Hydrogen Evolution

Liang

Lee

et al. 2023

Angewandte Chemie

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Efficient in situ deposition of metallic cocatalyst, like zero-valent platinum (Pt), on organic photovoltaic catalysts (OPCs) is the prerequisite for their high catalytic activities. Here we develop the OPC (Y6CO), by introducing carbonyl in the core, which is available to σ-π coordinate with transition metals, due to the highenergy empty π* orbital of carbonyl. Y6CO exhibits a stronger capability to anchor Pt species and reduce them to metallic state, resulting in more Pt 0 deposition, relative to the control OPC without the central σ-π anchor. Single-component and heterojunction nanoparticles (NPs) employing Y6CO show enhanced average hydrogen evolution rates of 230.98 and 323.22 mmol h À 1 g [OPC] À 1 , respectively, under AM 1.5G, 100 mW cm À 2 for 10 h, and heterojunction NPs yield the external quantum efficiencies of ca. 10 % in 500-800 nm. This work demonstrates that σ-π anchoring is one efficient strategy for integrating metallic cocatalyst and OPC for high-performance photocatalysis.

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“…Alternatively, two rigid nitrogen atoms in the BTD ring form hydrogen bonds with the adjacent atoms to improve the molecular backbone’s planarity [ 25 ]. Many BTD-containing polymers and small molecules have been widely used in several organic electronic applications, such as solar cells, organic light-emitting diodes (OLEDs), and organic field-effect transistors (OFETs) [ 26 , 27 , 28 ]. However, thiophene and oligothiophene derivates have been extensively studied as donor units for developing small organic molecules owing to their ease of synthesis, superb stability, and excellent hole/electron transport characteristics [ 29 , 30 , 31 ].…”

Section: Introductionmentioning

confidence: 99%

Linear-Shaped Low-Bandgap Asymmetric Conjugated Donor Molecule for Fabrication of Bulk Heterojunction Small-Molecule Organic Solar Cells

et al. 2023

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A linear–shaped small organic molecule (E)-4-(5-(3,5-dimethoxy-styryl)thiophen-2-yl)-7-(5’’-hexyl-[2,2’:5’,2’’-terthiophen]-5-yl)benzo[c][1,2,5]thiadiazole (MBTR) comprising a benzothiadiazole (BTD) acceptor linked with the terminal donors bithiophene and dimethoxy vinylbenzene through a π-bridge thiophene was synthesized and analyzed. The MBTR efficiently tuned the thermal, absorption, and emission characteristics to enhance the molecular packing and aggregation behaviors in the solid state. The obtained optical bandgap of 1.86 eV and low-lying highest occupied molecular orbital (HOMO) level of −5.42 eV efficiently lowered the energy losses in the fabricated devices, thereby achieving enhanced photovoltaic performances. The optimized MBTR:PC71BM (1:2.5 w/w%) fullerene-based devices showed a maximum power conversion efficiency (PCE) of 7.05%, with an open-circuit voltage (VOC) of 0.943 V, short-circuit current density (JSC) of 12.63 mA/cm2, and fill factor (FF) of 59.2%. With the addition of 3% 1,8-diiodooctane (DIO), the PCE improved to 8.76% with a high VOC of 1.02 V, JSC of 13.78 mA/cm2, and FF of 62.3%, which are associated with improved charge transport at the donor/acceptor interfaces owing to the fibrous active layer morphology and favorable phase separation. These results demonstrate that the introduction of suitable donor/acceptor groups in molecular design and device engineering is an effective approach to enhancing the photovoltaic performances of organic solar cells.

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Organic Photovoltaic Catalyst with Extended Exciton Diffusion for High-Performance Solar Hydrogen Evolution

Cited by 46 publications

References 68 publications

Construction of Efficient D–A-Type Photocatalysts by B–N Bond Substitution for Water Splitting

Construction of Efficient D–A-Type Photocatalysts by B–N Bond Substitution for Water Splitting

Organic Photovoltaic Catalyst with σ‐π Anchor for High‐Performance Solar Hydrogen Evolution

Linear-Shaped Low-Bandgap Asymmetric Conjugated Donor Molecule for Fabrication of Bulk Heterojunction Small-Molecule Organic Solar Cells

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