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  • Chemistry/Pharmacy  (38)
  • VA 2100  (38)
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  • Chemistry/Pharmacy  (38)
RVK
  • 1
    Online Resource
    Online Resource
    Electrocatalytic Urea Synthesis with 63.5 % Faradaic Efficiency and 100 % N‐Selectivity via One‐step C−N coupling
    Wiley ; 2023
    In:  Angewandte Chemie Vol. 135, No. 33 ( 2023-08-14)
    Details
    In: Angewandte Chemie, Wiley, Vol. 135, No. 33 ( 2023-08-14)
    Abstract: Electrocatalytic urea synthesis via coupling N 2 and CO 2 provides an effective route to mitigate energy crisis and close carbon footprint. However, the difficulty on breaking N≡N is the main reason that caused low efficiencies for both electrocatalytic NH 3 and urea synthesis, which is the bottleneck restricting their industrial applications. Herein, a new mechanism to overcome the inert of the nitrogen molecule was proposed by elongating N≡N instead of breaking N≡N to realize one‐step C−N coupling in the process for urea production. We constructed a Zn−Mn diatomic catalyst with axial chloride coordination, Zn−Mn sites display high tolerance to CO poisoning and the Faradaic efficiency can even be increased to 63.5 %, which is the highest value that has ever been reported. More importantly, negligible N≡N bond breakage effectively avoids the generation of ammonia as intermediates, therefore, the N‐selectivity in the co‐electrocatalytic system reaches100 % for urea synthesis. The previous cognition that electrocatalysts for urea synthesis must possess ammonia synthesis activity has been broken. Isotope‐labelled measurements and Operando synchrotron‐radiation Fourier transform infrared spectroscopy validate that activation of N−N triple bond and nitrogen fixation activity arise from the one‐step C−N coupling process of CO species with adsorbed N 2 molecules.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v135.33
    DOI: 10.1002/ange.202305447
    RVK:
    VA 2100
    RVK:
    VN 5020
    Language: English
    Publisher: Wiley
    Publication Date: 2023
    detail.hit.zdb_id: 505868-5
    detail.hit.zdb_id: 506609-8
    detail.hit.zdb_id: 514305-6
    detail.hit.zdb_id: 505872-7
    detail.hit.zdb_id: 1479266-7
    detail.hit.zdb_id: 505867-3
    detail.hit.zdb_id: 506259-7
    Location Call Number Limitation Availability
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    Online Resource
  • 2
    Online Resource
    Online Resource
    Electrocatalytic Urea Synthesis with 63.5 % Faradaic Efficiency and 100 % N‐Selectivity via One‐step C−N coupling
    Wiley ; 2023
    In:  Angewandte Chemie International Edition Vol. 62, No. 33 ( 2023-08-14)
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 62, No. 33 ( 2023-08-14)
    Abstract: Electrocatalytic urea synthesis via coupling N 2 and CO 2 provides an effective route to mitigate energy crisis and close carbon footprint. However, the difficulty on breaking N≡N is the main reason that caused low efficiencies for both electrocatalytic NH 3 and urea synthesis, which is the bottleneck restricting their industrial applications. Herein, a new mechanism to overcome the inert of the nitrogen molecule was proposed by elongating N≡N instead of breaking N≡N to realize one‐step C−N coupling in the process for urea production. We constructed a Zn−Mn diatomic catalyst with axial chloride coordination, Zn−Mn sites display high tolerance to CO poisoning and the Faradaic efficiency can even be increased to 63.5 %, which is the highest value that has ever been reported. More importantly, negligible N≡N bond breakage effectively avoids the generation of ammonia as intermediates, therefore, the N‐selectivity in the co‐electrocatalytic system reaches100 % for urea synthesis. The previous cognition that electrocatalysts for urea synthesis must possess ammonia synthesis activity has been broken. Isotope‐labelled measurements and Operando synchrotron‐radiation Fourier transform infrared spectroscopy validate that activation of N−N triple bond and nitrogen fixation activity arise from the one‐step C−N coupling process of CO species with adsorbed N 2 molecules.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v62.33
    DOI: 10.1002/anie.202305447
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2023
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
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    Online Resource
  • 3
    Online Resource
    Online Resource
    Green Solvent Processable, Asymmetric Dopant‐Free Hole Transport Layer Material for Efficient and Stable n‐i‐p Perovskite Solar Cells and Modules
    Wiley ; 2023
    In:  Angewandte Chemie International Edition Vol. 62, No. 46 ( 2023-11-13)
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 62, No. 46 ( 2023-11-13)
    Abstract: The use of dopant‐free hole transport layers (HTLs) is critical in stabilizing n‐i‐p perovskite solar cells (pero‐SCs). However, these HTL materials are often processed with toxic solvents, which is not ideal for industrial production. Upon substituting them with green solvents, a trade‐off emerges between maintaining the high crystallinity of the HTL materials and ensuring high solubility in the new solvents. In this paper, we designed a novel, linear, organic small molecule, BDT‐C8‐3O, by introducing an asymmetric polar oligo(ethylene glycol) side chain. This method not only overcomes the solubility limitations in green solvents but also enables stacking the conjugated main chains in two patterns, which further enhances crystallinity and hole mobility. As a result, the n ‐ i ‐ p pero‐SCs based on chlorobenzene‐ or green (natural compound) solvent 3‐methylcyclohexanone‐processed BDT‐C8‐3O HTL that without any dopant delivered world‐recorded power conversion efficiencies of 24.11 % (certified of 23.82 %) and 23.53 %, respectively. The devices also demonstrated remarkable operational and high‐temperature stabilities, maintaining over 84 % and 79.5 % of their initial efficiency for 2000 h, respectively. Encouragingly, dopant‐free BDT‐C8‐3O HTL exhibits significant advantages in large‐area fabrication, achieving state‐of‐the‐art PCEs exceeding 20 % for 5×5 cm 2 modules (active area: 15.64 cm 2 ), even when processed using green solvents.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v62.46
    DOI: 10.1002/anie.202312231
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2023
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
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    Online Resource
  • 4
    Online Resource
    Online Resource
    C‐Bound or O‐Bound Surface: Which One Boosts Electrocatalytic Urea Synthesis?
    Wiley ; 2023
    In:  Angewandte Chemie International Edition Vol. 62, No. 19 ( 2023-05-02)
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 62, No. 19 ( 2023-05-02)
    Abstract: The electrocatalytic C−N coupling from carbon dioxide and nitrate under ambient conditions is kind of sustainable and promising alternative method for urea synthesis. To date, the influence of catalyst surface properties on molecular adsorption configuration and electrocatalytic urea synthesis activity is unclear. In this work, we proposed that the urea synthesis activity is closely linked with the localized surface charge on bimetallic electrocatalysts, it is found that a negatively charged surface induces C‐bound path and boosts urea synthesis. The urea yield rate can reach 13.1 mmol g −1 h −1 on negatively charged Cu 97 In 3 ‐C, which is about 13 times that of positively charged Cu 30 In 70 ‐C counterpart with O‐bound surface. This conclusion also applies to Cu−Bi and Cu−Sn systems. The molecular modification shifts the surface of Cu 97 In 3 ‐C to positively charged state, which leads to a sharp decline in urea synthesis performance. We demonstrated that the C‐bound surface is more favorable than O‐bound one to boost electrocatalytic urea synthesis.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v62.19
    DOI: 10.1002/anie.202300387
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2023
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
    Location Call Number Limitation Availability
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    Online Resource
  • 5
    Online Resource
    Online Resource
    Green Solvent Processable, Asymmetric Dopant‐Free Hole Transport Layer Material for Efficient and Stable n‐i‐p Perovskite Solar Cells and Modules
    Wiley ; 2023
    In:  Angewandte Chemie Vol. 135, No. 46 ( 2023-11-13)
    Details
    In: Angewandte Chemie, Wiley, Vol. 135, No. 46 ( 2023-11-13)
    Abstract: The use of dopant‐free hole transport layers (HTLs) is critical in stabilizing n‐i‐p perovskite solar cells (pero‐SCs). However, these HTL materials are often processed with toxic solvents, which is not ideal for industrial production. Upon substituting them with green solvents, a trade‐off emerges between maintaining the high crystallinity of the HTL materials and ensuring high solubility in the new solvents. In this paper, we designed a novel, linear, organic small molecule, BDT‐C8‐3O, by introducing an asymmetric polar oligo(ethylene glycol) side chain. This method not only overcomes the solubility limitations in green solvents but also enables stacking the conjugated main chains in two patterns, which further enhances crystallinity and hole mobility. As a result, the n ‐ i ‐ p pero‐SCs based on chlorobenzene‐ or green (natural compound) solvent 3‐methylcyclohexanone‐processed BDT‐C8‐3O HTL that without any dopant delivered world‐recorded power conversion efficiencies of 24.11 % (certified of 23.82 %) and 23.53 %, respectively. The devices also demonstrated remarkable operational and high‐temperature stabilities, maintaining over 84 % and 79.5 % of their initial efficiency for 2000 h, respectively. Encouragingly, dopant‐free BDT‐C8‐3O HTL exhibits significant advantages in large‐area fabrication, achieving state‐of‐the‐art PCEs exceeding 20 % for 5×5 cm 2 modules (active area: 15.64 cm 2 ), even when processed using green solvents.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v135.46
    DOI: 10.1002/ange.202312231
    RVK:
    VA 2100
    RVK:
    VN 5020
    Language: English
    Publisher: Wiley
    Publication Date: 2023
    detail.hit.zdb_id: 505868-5
    detail.hit.zdb_id: 506609-8
    detail.hit.zdb_id: 514305-6
    detail.hit.zdb_id: 505872-7
    detail.hit.zdb_id: 1479266-7
    detail.hit.zdb_id: 505867-3
    detail.hit.zdb_id: 506259-7
    Location Call Number Limitation Availability
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    Online Resource
  • 6
    Online Resource
    Online Resource
    Iodonium Initiators: Paving the Air‐free Oxidation of Spiro‐OMeTAD for Efficient and Stable Perovskite Solar Cells
    Wiley ; 2024
    In:  Angewandte Chemie Vol. 136, No. 5 ( 2024-01-25)
    Details
    In: Angewandte Chemie, Wiley, Vol. 136, No. 5 ( 2024-01-25)
    Abstract: To date, perovskite solar cells (pero‐SCs) with doped 2,2′,7,7′‐tetrakis(N,N‐di‐p‐methoxyphenylamine)‐9,9′‐spirobifluorene (Spiro‐OMeTAD) hole transporting layers (HTLs) have shown the highest recorded power conversion efficiencies (PCEs). However, their commercialization is still impeded by poor device stability owing to the hygroscopic lithium bis(trifluoromethanesulfonyl)imide and volatile 4‐tert‐butylpyridine dopants as well as time‐consuming oxidation in air. In this study, we explored a series of single‐component iodonium initiators with strong oxidability and different electron delocalization properties to precisely manipulate the oxidation states of Spiro‐OMeTAD without air assistance, and the oxidation mechanism was clearly understood. Iodine (III) in the diphenyliodonium cation (IP + ) can accept a single electron from Spiro‐OMeTAD and forms Spiro‐OMeTAD⋅ + owing to its strong oxidability. Moreover, because of the coordination of the strongly delocalized TFSI − with Spiro‐OMeTAD⋅ + in a stable radical complex, the resulting hole mobility was 30 times higher than that of pristine Spiro‐OMeTAD. In addition, the IP‐TFSI initiator facilitated the growth of a homogeneous and pinhole‐free Spiro‐OMeTAD film. The pero‐SCs based on this oxidizing HTL showed excellent efficiencies of 25.16 % (certified: 24.85 % for 0.062‐cm 2 ) and 20.71 % for a 15.03‐cm 2 module as well as remarkable overall stability.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v136.5
    DOI: 10.1002/ange.202316183
    RVK:
    VA 2100
    RVK:
    VN 5020
    Language: English
    Publisher: Wiley
    Publication Date: 2024
    detail.hit.zdb_id: 505868-5
    detail.hit.zdb_id: 506609-8
    detail.hit.zdb_id: 514305-6
    detail.hit.zdb_id: 505872-7
    detail.hit.zdb_id: 1479266-7
    detail.hit.zdb_id: 505867-3
    detail.hit.zdb_id: 506259-7
    Location Call Number Limitation Availability
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    Online Resource
  • 7
    Online Resource
    Online Resource
    Iodonium Initiators: Paving the Air‐free Oxidation of Spiro‐OMeTAD for Efficient and Stable Perovskite Solar Cells
    Wiley ; 2024
    In:  Angewandte Chemie International Edition Vol. 63, No. 5 ( 2024-01-25)
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 63, No. 5 ( 2024-01-25)
    Abstract: To date, perovskite solar cells (pero‐SCs) with doped 2,2′,7,7′‐tetrakis(N,N‐di‐p‐methoxyphenylamine)‐9,9′‐spirobifluorene (Spiro‐OMeTAD) hole transporting layers (HTLs) have shown the highest recorded power conversion efficiencies (PCEs). However, their commercialization is still impeded by poor device stability owing to the hygroscopic lithium bis(trifluoromethanesulfonyl)imide and volatile 4‐tert‐butylpyridine dopants as well as time‐consuming oxidation in air. In this study, we explored a series of single‐component iodonium initiators with strong oxidability and different electron delocalization properties to precisely manipulate the oxidation states of Spiro‐OMeTAD without air assistance, and the oxidation mechanism was clearly understood. Iodine (III) in the diphenyliodonium cation (IP + ) can accept a single electron from Spiro‐OMeTAD and forms Spiro‐OMeTAD⋅ + owing to its strong oxidability. Moreover, because of the coordination of the strongly delocalized TFSI − with Spiro‐OMeTAD⋅ + in a stable radical complex, the resulting hole mobility was 30 times higher than that of pristine Spiro‐OMeTAD. In addition, the IP‐TFSI initiator facilitated the growth of a homogeneous and pinhole‐free Spiro‐OMeTAD film. The pero‐SCs based on this oxidizing HTL showed excellent efficiencies of 25.16 % (certified: 24.85 % for 0.062‐cm 2 ) and 20.71 % for a 15.03‐cm 2 module as well as remarkable overall stability.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v63.5
    DOI: 10.1002/anie.202316183
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2024
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
    Location Call Number Limitation Availability
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    Online Resource
  • 8
    Online Resource
    Online Resource
    C‐Bound or O‐Bound Surface: Which One Boosts Electrocatalytic Urea Synthesis?
    Wiley ; 2023
    In:  Angewandte Chemie Vol. 135, No. 19 ( 2023-05-02)
    Details
    In: Angewandte Chemie, Wiley, Vol. 135, No. 19 ( 2023-05-02)
    Abstract: The electrocatalytic C−N coupling from carbon dioxide and nitrate under ambient conditions is kind of sustainable and promising alternative method for urea synthesis. To date, the influence of catalyst surface properties on molecular adsorption configuration and electrocatalytic urea synthesis activity is unclear. In this work, we proposed that the urea synthesis activity is closely linked with the localized surface charge on bimetallic electrocatalysts, it is found that a negatively charged surface induces C‐bound path and boosts urea synthesis. The urea yield rate can reach 13.1 mmol g −1 h −1 on negatively charged Cu 97 In 3 ‐C, which is about 13 times that of positively charged Cu 30 In 70 ‐C counterpart with O‐bound surface. This conclusion also applies to Cu−Bi and Cu−Sn systems. The molecular modification shifts the surface of Cu 97 In 3 ‐C to positively charged state, which leads to a sharp decline in urea synthesis performance. We demonstrated that the C‐bound surface is more favorable than O‐bound one to boost electrocatalytic urea synthesis.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v135.19
    DOI: 10.1002/ange.202300387
    RVK:
    VA 2100
    RVK:
    VN 5020
    Language: English
    Publisher: Wiley
    Publication Date: 2023
    detail.hit.zdb_id: 505868-5
    detail.hit.zdb_id: 506609-8
    detail.hit.zdb_id: 514305-6
    detail.hit.zdb_id: 505872-7
    detail.hit.zdb_id: 1479266-7
    detail.hit.zdb_id: 505867-3
    detail.hit.zdb_id: 506259-7
    Location Call Number Limitation Availability
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    Online Resource
  • 9
    Online Resource
    Online Resource
    Generation of Fe IV =O and its Contribution to Fenton‐Like Reactions on a Single‐Atom Iron−N−C Catalyst
    Wiley ; 2023
    In:  Angewandte Chemie Vol. 135, No. 10 ( 2023-03)
    Details
    In: Angewandte Chemie, Wiley, Vol. 135, No. 10 ( 2023-03)
    Abstract: Generating Fe IV =O on single‐atom catalysts by Fenton‐like reaction has been established for water treatment; however, the Fe IV =O generation pathway and oxidation behavior remain obscure. Employing an Fe−N−C catalyst with a typical Fe−N 4 moiety to activate peroxymonosulfate (PMS), we demonstrate that generating Fe IV =O is mediated by an Fe−N−C−PMS* complex—a well‐recognized nonradical species for induction of electron‐transfer oxidation—and we determined that adjacent Fe sites with a specific Fe 1 −Fe 1 distance are required. After the Fe atoms with an Fe 1 ‐Fe 1 distance 〈 4 Å are PMS‐saturated, Fe−N−C−PMS* formed on Fe sites with an Fe 1 ‐Fe 1 distance of 4–5 Å can coordinate with the adjacent Fe II −N 4 , forming an inter‐complex with enhanced charge transfer to produce Fe IV =O. Fe IV =O enables the Fenton‐like system to efficiently oxidize various pollutants in a substrate‐specific, pH‐tolerant, and sustainable manner, where its prominent contribution manifests for pollutants with higher one‐electron oxidation potential.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v135.10
    DOI: 10.1002/ange.202218510
    RVK:
    VA 2100
    RVK:
    VN 5020
    Language: English
    Publisher: Wiley
    Publication Date: 2023
    detail.hit.zdb_id: 505868-5
    detail.hit.zdb_id: 506609-8
    detail.hit.zdb_id: 514305-6
    detail.hit.zdb_id: 505872-7
    detail.hit.zdb_id: 1479266-7
    detail.hit.zdb_id: 505867-3
    detail.hit.zdb_id: 506259-7
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  • 10
    Online Resource
    Online Resource
    Rhodium‐Catalyzed Reaction of Silacyclobutanes with Unactivated Alkynes to Afford Silacyclohexenes
    Wiley ; 2019
    In:  Angewandte Chemie Vol. 131, No. 14 ( 2019-03-26), p. 4743-4747
    Details
    In: Angewandte Chemie, Wiley, Vol. 131, No. 14 ( 2019-03-26), p. 4743-4747
    Abstract: A Rh‐catalyzed reaction of silacyclobutanes (SCBs) with unactivated alkynes has been developed to form silacyclohexenes with high chemoselectivity. Good enantioselectivity at the stereogenic silicon center was achieved using a chiral phosphoramidite ligand. The resulting silacyclohexenes are useful scaffolds for synthesizing structurally attractive silacyclic compounds.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v131.14
    DOI: 10.1002/ange.201814143
    RVK:
    VA 2100
    RVK:
    VN 5020
    Language: English
    Publisher: Wiley
    Publication Date: 2019
    detail.hit.zdb_id: 505868-5
    detail.hit.zdb_id: 506609-8
    detail.hit.zdb_id: 514305-6
    detail.hit.zdb_id: 505872-7
    detail.hit.zdb_id: 1479266-7
    detail.hit.zdb_id: 505867-3
    detail.hit.zdb_id: 506259-7
    Location Call Number Limitation Availability
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