Structure evolution of thiophene-containing conjugated polymer photocatalysts for high-efficiency photocatalytic hydrogen production

Xiang, Sihui; Han, Changzhi; Zhang, Chong; Jiang, Jia‐Xing

doi:10.1007/s40843-021-1757-1

Cited by 31 publications

(15 citation statements)

References 57 publications

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“…Previous studies revealed that the sacrificial agents also have a large influence on the photocatalytic activity of conjugated polymer photocatalysts. [37][38][39] Therefore, we further investigated the photocatalytic activity of DBC-BTDO by adopting other two common sacrificial agents of triethanolamine (TEOA) and triethylamine (TEA). The bare polymer of DBC-BTDO could still exhibit a high photocatalytic activity with the HERs of 37.35 and 29.14 mmol h -1 g -1 when using TEOA and TEA as the sacrificial agents, respectively (Figure 6b; Figure S10, Supporting Information).…”

Section: Resultsmentioning

confidence: 99%

An Efficient Electron Donor for Conjugated Microporous Polymer Photocatalysts with High Photocatalytic Hydrogen Evolution Activity

Han

Xiang

et al. 2022

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electronic structure. [3][4][5] Nevertheless, most inorganic photocatalysts suffer from low activity under visible light, complexity in the preparation, and the limited natural resources. Recent studies demonstrated that organic semiconductors could be a promising class of photocatalysts for hydrogen evolution because of their diverse structures, various synthetic strategies, and tunable electronic properties. [6][7][8] To date, various organic polymers with conjugated skeletons have been developed as photocatalysts for hydrogen evolution. [9][10][11] In particular, significant advances in the preparation of conjugated microporous polymer (CMP) photocatalysts with high photocatalytic activity have been achieved. [12][13][14] Many studies revealed that designing a donor-acceptor (D-A) molecular structure is an efficient strategy to boost the photocatalytic activity of conjugated polymer photocatalysts, [15][16][17][18] since the intrinsic electron push-pull effect in a D-A conjugated polymer could promote the separation of light-induced hole/ electron. The nature of electron donor and acceptor units plays a key point in the charges transfer and separation, which affect significantly the photocatalytic activity. Therefore, the selection of electron donor and acceptor is of great importance for constructing organic polymer photocatalysts with high photocatalytic activity. In general, aromatic heterocyclic compounds with narrow band gap are commonly used as electron acceptors, and aromatic hydrocarbons with delocalized π-electron are employed as electron donors to build D-A type polymer photocatalysts. Based on the developed D-A polymer photo catalysts to date, [15,[19][20][21][22] dibenzo[b,d]thiophene-S,S-dioxide (BTDO) might be the most effective acceptor unit due to its strong electronwithdrawing capability and high hydrophilicity, [23][24][25] and pyrene with planar molecular structure and large delocalized π-electron system is the most effective electron donor to prepare high performance polymer photocatalysts. [26,27] Although there have been significant advances in the photo catalytic activity of polymer photocatalysts by structure optimization, [28,29] the limited scope of high efficient electron donors and acceptors hinders the further development of organic polymer photo catalysts. To further improve the photocatalytic activity and enrich the D-A) molecular structure show high photocatalytic activity for hydrogen evolution due to the efficient light-induced electron/hole separation, which is mostly determined by the nature of electron donor and acceptor units. Therefore, the selection of electron donor and acceptor holds the key point to construct high performance polymer photocatalysts. Herein, two dibenzo[b,d]thiophene-S,Sdioxide (BTDO) containing CMP photocatalysts using tetraphenylethylene (TPE) or dibenzo[g,p]chrysene (DBC) as the electron donor to investigate the influence of the geometry of electron donor on the photocatalytic activity are design and synthesized. Compared with the twisted TPE donor,...

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Section: Resultsmentioning

confidence: 99%

An Efficient Electron Donor for Conjugated Microporous Polymer Photocatalysts with High Photocatalytic Hydrogen Evolution Activity

Han

Xiang

et al. 2022

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“…To upgrade the photocatalytic activity of organic photocatalysts with conjugated frameworks, various strategies have been put forward, such as expanding the optical absorption range, − designing organic–inorganic or organic–organic heterojunctions, − constructing donor–acceptor (D–A) or donor−π–acceptor (D−π–A) structures − and enhancing the hydrophilicity. − Among these strategies, building D–A or D−π–A type polymer photocatalysts has attracted great attention, since the intrinsic electron push–pull effect between donor units and acceptor units is advantageous in facilitating the photo-induced charge separation and thus increasing the photocatalytic activity of the polymer photocatalysts. For example, Li and co-workers developed a D–A type porous organic photocatalyst of BTT-CPP with conjugated frameworks using benzo[1,2- b :3,4- b ′:5,6- b ″]trithiophene as the electron donor and BTDO as the electron acceptor.…”

Section: Introductionmentioning

confidence: 99%

Rational Design of Conjugated Microporous Polymer Photocatalysts with Definite D−π–A Structures for Ultrahigh Photocatalytic Hydrogen Evolution Activity under Natural Sunlight

et al. 2022

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Organic polymers with conjugated architectures have been widely exploited as photocatalyst materials for hydrogen generation. However, it is still an enormous challenge to develop photocatalysts with high hydrogen generation activity under natural sunlight, which is pretty significant for practical applications. Herein, two conjugated microporous polymer photocatalysts with definite D−π–A structures are designed and prepared using dibenzo[g,p]chrysene or pyrene with planar conjugated architecture as electron donors, thiophene as a π-spacer, and dibenzo[b,d]thiophene-S,S-dioxide as an electron acceptor. Benefiting from the efficient separation of light-generated electrons/holes due to the definite D−π–A structure and the broad light absorption range, the bare polymer Py-TP-BTDO could deliver a high photocatalytic hydrogen evolution rate (HER) of 115.03 mmol h–1 g–1 upon exposure to visible light (λ > 420 nm). Impressively, the outdoor photocatalytic experiment reveals that abundant and continuous hydrogen bubbles could be produced fast and visually observed under natural sunlight by the Py-TP-BTDO polymer film with a large active area of 120 cm2. A water-drainage experiment further demonstrates that 1224 mL of hydrogen gas could be produced by 25 mg of a polymer photocatalyst with 3 wt % Pt cocatalyst under natural sunlight in 7 h, corresponding to a high HER of 312.24 mmol h–1 g–1, which represents the state of the art of organic photocatalyst materials to date. The high photocatalytic activity under natural sunlight suggests the potential of the developed Py-TP-BTDO polymer photocatalyst in the practical applications for photocatalytic hydrogen production.

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“…Due to these properties, the PyTP-2 (38) polymers generate 33.07 mmol g À 1 h À 1 H 2 and 58.37 mmol g À 1 h À 1 for O 2 evolution. [97] The comparison of various planarized conjugated polymers for hydrogen evolution is presented in Table 2. It can be concluded from Table 2 that choosing the correct material having photoactive functional groups, and combining it with TiO 2 , Cu, etc.…”

Section: R E V I E W T H E C H E M I C a L R E C O R Dmentioning

confidence: 99%

“…On the other hand, the planner molecular structure of polymer for both the donor and acceptor units enables the charge transmission along the D−A type polymer skeleton to dissociate the photoinduced electron and holes. Due to these properties, the PyTP‐2 ( 38 ) polymers generate 33.07 mmol g −1 h −1 H 2 and 58.37 mmol g −1 h −1 for O 2 evolution [97] . The comparison of various planarized conjugated polymers for hydrogen evolution is presented in Table 2.…”

Section: Conjugated Polymers For Photocatalytic H2o Splittingmentioning

confidence: 99%

Photocatalytic Water‐Splitting by Organic Conjugated Polymers: Opportunities and Challenges

Mansha

Ahmad

Khan

et al. 2022

The Chemical Record

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The future challenges associated with the shortage of fossil fuels and their current environmental impacts intrigued the researchers to look for alternative ways of generating green energy. Solar‐driven water splitting into oxygen and hydrogen is one of those advanced strategies. Researchers have studied various semiconductor materials to achieve potential results. However, it encountered multiple challenges such as high cost, low photostability and efficiency, and required multistep modifications. The conjugated polymers (CPs) have emerged as promising alternatives for conventional inorganic semiconductors. The CPs offer low cost, sufficient light absorption efficiency, excellent photo and chemical stability, and molecular optoelectronic tunable characteristics. Furthermore, organic CPs also present higher flexibility to tune the basic framework of the backbone of the polymers, amendments in the sidechain to incorporate desired functionalities, and much‐needed porosity to serve better for photocatalytic applications. This review article summarizes the recent advancements made in visible‐light‐driven water splitting covering the aspects of synthetic strategies and experimental parameters employed for water splitting reactions with special emphasis on conjugated polymers such as linear CPs, planarized CPs, graphitic carbon nitride (g‐C3N4), conjugated microporous polymers (CMPs), covalent organic frameworks (COFs), and conjugated polymer‐based nanocomposites (CPNCs). The current challenges and future prospects have also been described briefly.

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Structure evolution of thiophene-containing conjugated polymer photocatalysts for high-efficiency photocatalytic hydrogen production

Cited by 31 publications

References 57 publications

An Efficient Electron Donor for Conjugated Microporous Polymer Photocatalysts with High Photocatalytic Hydrogen Evolution Activity

An Efficient Electron Donor for Conjugated Microporous Polymer Photocatalysts with High Photocatalytic Hydrogen Evolution Activity

Rational Design of Conjugated Microporous Polymer Photocatalysts with Definite D−π–A Structures for Ultrahigh Photocatalytic Hydrogen Evolution Activity under Natural Sunlight

Photocatalytic Water‐Splitting by Organic Conjugated Polymers: Opportunities and Challenges

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