Atomic Sandwiched p‐n Homojunctions

Wu, Yu; Liu, Xiaoqing; Zhang, Huijuan; Li, Jian; Zhou, Miao; Li, Liang; Wang, Yu

doi:10.1002/anie.202012734

Cited by 41 publications

(34 citation statements)

References 57 publications

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“…The separation efficiency (η sep ) in Figure 4a was measured to estimate the photo-generated carrier recombination inner the photoanode, [36] which can be calculated by the following equation:…”

Section: Resultsmentioning

confidence: 99%

“…The separation efficiency (η sep ) in Figure 4 a was measured to estimate the photo‐generated carrier recombination inner the photoanode, [ 36 ] which can be calculated by the following equation:

\begin{matrix} η_{sep} = J_{sulfite} / J_{abs} \end{matrix}

where J sulfite in Figure S17, Supporting Information, is the net photocurrent density measured in hole scavenger (0.5 m Na 2 SO 3 /NaH 2 PO 4 , pH = 7.5) and J abs is calculated from the UV–vis data and standard AM 1.5G solar spectrum. UV–vis spectra in Figure S18a, Supporting Information, can be applied to reveal the light absorption performance of photoanodes.…”

Section: Resultsmentioning

confidence: 99%

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Incorporation of Sulfate Anions and Sulfur Vacancies in ZnIn₂S₄ Photoanode for Enhanced Photoelectrochemical Water Splitting

Gao

Meng

et al. 2021

Advanced Energy Materials

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105

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friendly properties. [6] However, due to its severe bulk carrier recombination, unfavorable carrier transportation, and sluggish surface OER dynamics, the PEC performance of bare ZnIn 2 S 4 photoanode is still not satisfactory.Various strategies have been developed to enhance the PEC performance of ZnIn 2 S 4 , such as morphology engineering, constructing heterojunctions, and coating surface co-catalysts, etc. [7][8][9] Among them, decorating surface cocatalysts has been considered as an effective strategy to promote surface water oxidation kinetics of pristine ZnIn 2 S 4 . However, the integration of water-oxidation cocatalysts with PEC photoanodes has been limited to metal-based materials, such Co-Pi, FeCoO x , and FeOOH. [10][11][12][13][14][15] The cocatalysts containing metallic ions tend to be toxic and expensive, which could limit their further applications. In addition, these cocatalysts may cause light absorption attenuation and increased charge recombination due to the large thickness/dimension of cocatalysts and additional interface defects between cocatalysts and photo anodes. Recently, nonmetallic anionic groups, such as phosphate (PO 4 3− ), selenate (SeO 4 2− ), and sulfate (SO 4 2− ), have emerged as alternatives to boost water oxidation ability. [16][17][18] These nonmetallic groups could optimize the electronic structure of active sites, regulate the adsorption of intermediates to reduce OER overpotential, and promote the surface carrier transfer. Particularly, the SO 4 2− group can break the adsorption-energy scaling relation between OH* and OOH* (reaction intermediates) and decrease the OER overpotential. [17] Accordingly, engineering ZnIn 2 S 4 with SO 4 2− groups is a promising strategy to improve its surface reaction kinetics. However, the introduction of nonmetallic anionic groups usually relies on a direct mixing method or external addition, which leads to weak chemical interaction and thus decreases the effectiveness and durability of the resultant materials. [17] In contrast, in situ introducing SO 4 2− anionic groups into ZnIn 2 S 4 to induce strong bonding between anions and metal atoms is expected to remarkably facilitate solar water oxidation.As a kind of intrinsic defect for metal sulfide, sulfur vacancies (S v ) have the ability to adjust the electronic structure of metal sulfide, leading to optimization of the adsorption free energy and also improvement of the conductivity. [19,20] S v can be divided into bulk S v and surface S v according to their spatial Severe charge recombination and slow surface water oxidation kinetics seriously limit the practical application of ZnIn 2 S 4 photoanodes for photo electrochemical water splitting. Herein, an in situ strategy to introduce sulfate (SO 4 2− ) anions and controlled bulk sulfur vacancies (S v ) into a ZnIn 2 S 4 photoanode is developed, and its PEC performance is remarkably enhanced, achieving a photocurrent density of 3.52 mA cm −2 at 1.23 V versus reversible hydrogen electrode (V RHE ) and negatively shifted onset potential of 0....

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Section: Resultsmentioning

confidence: 99%

\begin{matrix} η_{sep} = J_{sulfite} / J_{abs} \end{matrix}

Section: Resultsmentioning

confidence: 99%

Incorporation of Sulfate Anions and Sulfur Vacancies in ZnIn₂S₄ Photoanode for Enhanced Photoelectrochemical Water Splitting

Gao

Meng

et al. 2021

Advanced Energy Materials

Self Cite

105

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“…Previously, hydroarylation reactions of unconjugated double bonds of alkenyl alcohols have been realized using a palladium‐catalyzed redox‐relay strategy [6] . Very recently, a nickel‐catalyzed hydroarylation strategy between a double bond remote from a carbonyl group and arylboronic acid has been disclosed [7] . Unfortunately, redox‐neutral hydroarylation of double bonds out of conjugation with a carbonyl group remains a challenge in the field of palladium catalysis.…”

Section: Introductionmentioning

confidence: 99%

DFT Mechanistic Study on Palladium‐Catalyzed Redox‐Neutral Hydroarylation of Unactivated Alkenes with Arylboronic Acids

Zhou

et al. 2021

Asian J Org Chem

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Density functional calculations were carried out on the mechanism of a palladium‐catalyzed hydroarylation reaction of β,γ‐unsaturated carbonyl compounds with arylboronic acids reported by Engle's group. The proposed reaction pathway consists of several key mechanistic steps, including the chelation of substrate 1 a, transmetalation of organoboron 2 a, migratory insertion, protodepalladation, and dechelation of product 3 a, among which the transmetalation step is rate‐determining with a free‐energy barrier of 27.0 kcal/mol. Experimental researchers proposed that the chelation of Daugulis's 8‐aminoquinoline (AQ) directing group facilitated the desired hydroarylation in a γ‐selective manner. However, the present study revealed that the chelation of AQ indeed retarded the delivery of the aryl group to the double bond and the regioselectivity was not necessarily the result of this group. Indeed, it could effectively prevent the homocoupling of 2 a, because the homocoupling was predicted to be easier than the desired hydroarylation in the absence of AQ. Additionally, some reductive coupling pathways between 1 a and 2 a were designed, and the competition of them was discussed in great detail. Lastly, the extension of this synthetic strategy to other types of alkenes was predicted.

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“…Zhang et al. recently reported the elegant enantioselective intermolecular radical C−H amination, [27d] and we [27c] and Liu [27e] independently developed asymmetric carboazidation of styrenes and acrylamides. Despite these recent breakthroughs, asymmetric aminoazidation and diazidation remain important unsolved problems.…”

Section: Introductionmentioning

confidence: 99%

Iron‐Catalyzed Radical Asymmetric Aminoazidation and Diazidation of Styrenes

Sun

Zhou

et al. 2021

Angewandte Chemie

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Asymmetric aminoazidation and diazidation of alkenes are straightforward strategies to build value‐added chiral nitrogen‐containing compounds from feedstock chemicals. They provide direct access to chiral organoazides and complement enantioselective diamination. Despite the advances in non‐asymmetric reactions, asymmetric aminoazidation or diazidation based on acyclic systems has not been previously reported. Here we describe the iron‐catalyzed intermolecular asymmetric aminoazidation and diazidation of styrenes. The method is practically useful and requires relatively low loading of catalyst and chiral ligand. With mild reaction conditions, the reaction can be completed on a 20 mmol scale. Studies of the mechanism suggest that the reaction proceeds via a radical pathway and involves stereocontrol of an acyclic free radical which probably takes place through a group transfer mechanism.

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Atomic Sandwiched p‐n Homojunctions

Cited by 41 publications

References 57 publications

Incorporation of Sulfate Anions and Sulfur Vacancies in ZnIn₂S₄ Photoanode for Enhanced Photoelectrochemical Water Splitting

Incorporation of Sulfate Anions and Sulfur Vacancies in ZnIn₂S₄ Photoanode for Enhanced Photoelectrochemical Water Splitting

DFT Mechanistic Study on Palladium‐Catalyzed Redox‐Neutral Hydroarylation of Unactivated Alkenes with Arylboronic Acids

Iron‐Catalyzed Radical Asymmetric Aminoazidation and Diazidation of Styrenes

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Atomic Sandwiched p‐n Homojunctions

Cited by 41 publications

References 57 publications

Incorporation of Sulfate Anions and Sulfur Vacancies in ZnIn2S4 Photoanode for Enhanced Photoelectrochemical Water Splitting

Incorporation of Sulfate Anions and Sulfur Vacancies in ZnIn2S4 Photoanode for Enhanced Photoelectrochemical Water Splitting

DFT Mechanistic Study on Palladium‐Catalyzed Redox‐Neutral Hydroarylation of Unactivated Alkenes with Arylboronic Acids

Iron‐Catalyzed Radical Asymmetric Aminoazidation and Diazidation of Styrenes

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Resources

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Incorporation of Sulfate Anions and Sulfur Vacancies in ZnIn₂S₄ Photoanode for Enhanced Photoelectrochemical Water Splitting

Incorporation of Sulfate Anions and Sulfur Vacancies in ZnIn₂S₄ Photoanode for Enhanced Photoelectrochemical Water Splitting