Efficient hydrogen peroxide synthesis by metal-free polyterthiophene <i>via</i> photoelectrocatalytic dioxygen reduction

Fan, Wenjun; Zhang, Bingqing; Wang, Xiaoyu; Ma, Weiguang; Deng, Li; Wang, Zhiliang; Dupuis, Michel; Shi, Jingying; Liao, Shijun; Li, Can

doi:10.1039/c9ee02247c

Cited by 176 publications

(145 citation statements)

References 43 publications

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“…In this design, CTF layers can be conveniently synthesized via electropolymerization which is an inexpensive, fast and effective approach for the growth of thin films of conductive polymers. [38,39] The overall preparation route is schematically shown in Figure 1a. The UV-vis-NIR diffuse reflectance spectrum of CTF-BTh is shown in Figure S1 in the Supporting Information.…”

Section: Resultsmentioning

confidence: 99%

Stable Unbiased Photo‐Electrochemical Overall Water Splitting Exceeding 3% Efficiency via Covalent Triazine Framework/Metal Oxide Hybrid Photoelectrodes

Zhang

et al. 2021

Advanced Materials

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Photo‐electrochemical (PEC) water splitting systems using oxide‐based photoelectrodes are highly attractive for solar‐to‐chemical energy conversion. However, despite decades‐long efforts, it is still challenging to develop efficient and stable photoelectrodes for practical applications. Here, thin layers of covalent triazine frameworks (CTF‐BTh) containing a bithiophene moiety are conformably deposited onto the surfaces of a Cu2O photocathode and a Mo‐doped BiVO4 photoanode via electropolymerization to construct new hybrid photoelectrodes, successfully addressing the efficiency and stability issues. The CTF‐BTh possesses a suitable band structure to form favorable band edge alignment with each metal oxide, creating a p–n junction and a staggered type‐II heterojunction with Cu2O and Mo‐doped BiVO4, respectively. Thus, the as‐fabricated hybrid photoelectrodes exhibit substantially increased PEC performances. Meanwhile, the CTF‐BTh film also serves as an effective corrosion‐resistant overlayer for both photoelectrodes to inhibit photocorrosion and enable long‐term operation for 150 h with only ≈10% loss in photocurrent densities. Furthermore, a stand‐alone unbiased PEC tandem device comprising CTF‐BTh‐coated photoelectrodes exhibits 3.70% solar‐to‐hydrogen conversion efficiency. Even after continuous operation for 120 h, the efficiency can still retain at 3.24%.

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Section: Resultsmentioning

confidence: 99%

Stable Unbiased Photo‐Electrochemical Overall Water Splitting Exceeding 3% Efficiency via Covalent Triazine Framework/Metal Oxide Hybrid Photoelectrodes

Zhang

et al. 2021

Advanced Materials

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“…[5,23,50,51] However, due to thermodynamical unfavorable water oxidative H 2 O 2 process, the FE still has a considerable room to improve as compared to the O 2 reductive H 2 O 2 in PEC system. [3,[52][53][54][55] Further development of strategies to suppress the decomposition of H 2 O 2 under given operating conditions and improve the PEC efficiency of BiVO 4 based photoanode will be the topic of a follow-up study.…”

Section: Resultsmentioning

confidence: 99%

Suppressing Water Dissociation via Control of Intrinsic Oxygen Defects for Awakening Solar H₂O‐to‐H₂O₂ Generation

Wang

Lü

Han

et al. 2021

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“…[ 25–27 ] The key factor determining which mechanism preferentially occurs during the ORR is the interaction strength of the hydrogen peroxide intermediate (H 2 O 2 or HO 2 − ) with the electrode surface. If the peroxide intermediate binds weakly to the electrode surface, as observed for metal‐free organic molecules, [ 20,28,29 ] the rate of desorption is higher than the electro‐reduction of peroxide and the reaction terminates at the two‐electron pathway. If peroxide binds strongly, the electro‐reduction of peroxide is expected to occur faster than desorption and the reaction terminates at the 4‐electron pathway.…”

Section: Figurementioning

confidence: 99%

Energetic Control of Redox‐Active Polymers toward Safe Organic Bioelectronic Materials

et al. 2020

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Organic semiconductors with polar sidechains have been identified as a promising class of materials for the field of bioelectronics. These materials, also called organic mixed ionic/electronic conductors (OMIECs), can exchange ions with aqueous electrolytes when electronic charge carriers are injected, transported, and stored in the bulk of the material. [1] Recent developments of OMIECs based on redox-active conjugated polymers [2][3][4][5][6][7][8] and novel device concepts [9,10] have opened up new pathways for bioelectronic devices including integrated circuits for electroencephalogram (EEG) monitoring [9] or low-power voltage amplifiers based on organic electrochemical transistors (OECTs). [11] Specifically, the OECT has drawn significant attention in the field of organic bioelectronics. It operates by electrochemically modulating the conductivity of a redox-active channel material with an electrolyte that is often aqueous, Avoiding faradaic side reactions during the operation of electrochemical devices is important to enhance the device stability, to achieve low power consumption, and to prevent the formation of reactive side-products. This is particularly important for bioelectronic devices, which are designed to operate in biological systems. While redox-active materials based on conducting and semiconducting polymers represent an exciting class of materials for bioelectronic devices, they are susceptible to electrochemical side-reactions with molecular oxygen during device operation. Here, electrochemical side reactions with molecular oxygen are shown to occur during organic electrochemical transistor (OECT) operation using high-performance, state-of-the-art OECT materials. Depending on the choice of the active material, such reactions yield hydrogen peroxide (H 2 O 2 ), a reactive side-product, which may be harmful to the local biological environment and may also accelerate device degradation. A design strategy is reported for the development of redox-active organic semiconductors based on donor-acceptor copolymers that prevents the formation of H 2 O 2 during device operation. This study elucidates the previously overlooked side-reactions between redox-active conjugated polymers and molecular oxygen in electrochemical devices for bioelectronics, which is critical for the operation of electrolyte-gated devices in application-relevant environments.

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Efficient hydrogen peroxide synthesis by metal-free polyterthiophene via photoelectrocatalytic dioxygen reduction

Abstract: We demonstrate the metal-free polymeric semiconductor pTTh as a selective and efficient photocathode for photoelectrochemical oxygen reduction to a high concentration of H2O2 in a cost-effective way.

Cited by 176 publications

References 43 publications

Stable Unbiased Photo‐Electrochemical Overall Water Splitting Exceeding 3% Efficiency via Covalent Triazine Framework/Metal Oxide Hybrid Photoelectrodes

Stable Unbiased Photo‐Electrochemical Overall Water Splitting Exceeding 3% Efficiency via Covalent Triazine Framework/Metal Oxide Hybrid Photoelectrodes

Suppressing Water Dissociation via Control of Intrinsic Oxygen Defects for Awakening Solar H₂O‐to‐H₂O₂ Generation

Energetic Control of Redox‐Active Polymers toward Safe Organic Bioelectronic Materials

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Efficient hydrogen peroxide synthesis by metal-free polyterthiophene via photoelectrocatalytic dioxygen reduction

Abstract: We demonstrate the metal-free polymeric semiconductor pTTh as a selective and efficient photocathode for photoelectrochemical oxygen reduction to a high concentration of H2O2 in a cost-effective way.

Cited by 176 publications

References 43 publications

Stable Unbiased Photo‐Electrochemical Overall Water Splitting Exceeding 3% Efficiency via Covalent Triazine Framework/Metal Oxide Hybrid Photoelectrodes

Stable Unbiased Photo‐Electrochemical Overall Water Splitting Exceeding 3% Efficiency via Covalent Triazine Framework/Metal Oxide Hybrid Photoelectrodes

Suppressing Water Dissociation via Control of Intrinsic Oxygen Defects for Awakening Solar H2O‐to‐H2O2 Generation

Energetic Control of Redox‐Active Polymers toward Safe Organic Bioelectronic Materials

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Suppressing Water Dissociation via Control of Intrinsic Oxygen Defects for Awakening Solar H₂O‐to‐H₂O₂ Generation