Structure of the Au23−xAgx(S‐Adm)15 Nanocluster and Its Application for Photocatalytic Degradation of Organic Pollutants

Liu, Chao; Ren, Xiaobing; Lin, Feng; Fu, Xuemei; Lin, Xin; Li, Tao; Sun, Keju; Huang, Jiahui

doi:10.1002/anie.201904612

Cited by 69 publications

(76 citation statements)

References 51 publications

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“…The electrocatalytic CO 2 reduction reaction (CO 2 RR) that enables the conversion of CO 2 into fuels or value-added organic compounds, along with the storage of intermittent electrical energy, and mitigates the environmental problem, has been regarded as a promising approach to meet future energy demands. [1][2][3][4] However, the uncontrolled multiple coupling processes of electron/protons in CO 2 RR lead to various reaction pathways, which always generate a number of different products, causing low faradaic efficiency (FE) and selectivity. [5][6][7] In addition, from the perspective of reaction thermodynamics, the equilibrium potentials for most CO 2 RR half-reactions (e.g.…”

Section: Introductionmentioning

confidence: 99%

Polyoxometalate-based electron transfer modulation for efficient electrocatalytic carbon dioxide reduction

Lang

et al. 2020

Chem. Sci.

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The electrocatalytic carbon dioxide (CO 2 ) reduction reaction (CO 2 RR) involves a variety of electron transfer pathways, resulting in poor reaction selectivity, limiting its use to meet future energy requirements.Polyoxometalates (POMs) can both store and release multiple electrons in the electrochemical process, and this is expected to be an ideal "electron switch" to match with catalytically active species, realize electron transfer modulation and promote the activity and selectivity of the electrocatalytic CO 2 RR.Herein, we report a series of new POM-based manganese-carbonyl (MnL) composite CO 2 reduction electrocatalysts, whereby SiW 12 -MnL exhibits the most remarkable activity and selectivity for CO 2 RR to CO, resulting in an increase in the faradaic efficiency (FE) from 65% (MnL) to a record-value of 95% in aqueous electrolyte. A series of control electrochemical experiments, photoluminescence spectroscopy (PL), transient photovoltage (TPV) experiments, and density functional theory (DFT) calculations revealed that POMs act as electronic regulators to control the electron transfer process from POM to MnL units during the electrochemical reaction, enhancing the selectivity of the CO 2 RR to CO and depressing the competitive hydrogen evolution reaction (HER). This work demonstrates the significance of electron transfer modulation in the CO 2 RR and suggests a new idea for the design of efficient electrocatalysts towards CO 2 RR.The preparation process of CsPOM/KB was as follows. Taking CsSiW 12 as an example, 0.08 g Cs 4 [a-SiW 12 O 40 ]$nH 2 O and 20 mg KB were mixed in 10 mL of aqueous solution uniformly by ultrasound for 1 hour. Then, the suspension was separated by centrifugation, washed with water three times, and dried in air. The obtained powder was denoted as CsSiW 12 /KB. CsPW 12 /KB and CsPMo 12 /KB were prepared in the same way. 3008 | Chem. Sci., 2020, 11, 3007-3015This journal is

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Section: Introductionmentioning

confidence: 99%

Polyoxometalate-based electron transfer modulation for efficient electrocatalytic carbon dioxide reduction

Lang

et al. 2020

Chem. Sci.

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“…The stability of the cluster can be remained, as confirmed by the compared IR and UV/Vis spectra (Supporting Information, Figure S21) of sample before and after photocatalysis. Noticeably, the photocatalytic activity of 1 is comparable to that of Au 23 (S‐Adm) 15 (HS‐Adm=adamantanethiol) NC, which degraded the RhB dye by 83 % after visible‐light irradiation for 40 min …”

Section: Figurementioning

confidence: 88%

A Sodalite‐Type Silver Orthophosphate Cluster in a Globular Silver Nanocluster

et al. 2020

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The synthesis and structure of a giant 102‐silver‐atom nanocluster (NC) 1 is presented. X‐ray structural analysis reveals that 1 features a multi‐shelled metallic core of Ag6@Ag24@Ag60@Ag12. An octahedral Ag6 core is encaged by a truncated octahedral Ag24 shell. The Ag24 shell is composed of a hitherto unknown sodalite‐type silver orthophosphate cluster (SOC) {(Ag3PO4)8}, reminiscent of the Ag3PO4 photocatalyst. The SOC is capped by six interstitial sulfur atoms, giving a unique anionic cluster [Ag6@{(Ag3PO4)8}S6]6−, which functions as an intricate polyhedral template with abundant surface O and S atoms guiding the formation of a rare rhombicosidodecahedral Ag60 shell. An array of 6 linear Ag2 staples further surround this Ag60 shell. [Ag6@{(Ag3PO4)8}S6]6− is an unusual Ag‐based templating anion to induce the assembly of a SOC within silver NC. This finding provides molecular models for bulk Ag3PO4, and offers a fresh template strategy for the synthesis of silver NCs with high symmetry.

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“…However, most of the conventional treatments for environment remediation were found inefficient and may cause secondary pollution. In recent years, sunlight-driven photocatalysis technology is considered to be a green, effective and economic method to handle the removal of environmental pollutions [182][183][184][185][186][187]. To date, tremendous efforts have been contributed to developing efficient photocatalysts to match the requirements of practical application [188][189][190][191].…”

Section: Removal Of Pollutionsmentioning

confidence: 99%

2D/2D heterostructured photocatalyst: Rational design for energy and environmental applications

2020

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Two-dimensional/two-dimensional (2D/2D) hybrid nanomaterials have triggered extensive research in the photocatalytic field. The construction of emerging 2D/2D heterostructures can generate many intriguing advantages in exploring high-performance photocatalysts, mainly including preferable dimensionality design allowing large contact interface area, integrated merits of each 2D component and rapid charge separation by the heterojunction effect. Herein, we provide a comprehensive review of the recent progress on the fundamental aspects, general synthesis strategies (in situ growth and ex situ assembly) of 2D/2D heterostructured photocatalysts and highlight their applications in the fields of hydrogen evolution, CO 2 reduction and removal of pollutants. Furthermore, the perspectives on the remaining challenges and future opportunities regarding the development of 2D/2D heterostructure photocatalysts are also presented.

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Structure of the Au_23−xAg_x(S‐Adm)₁₅ Nanocluster and Its Application for Photocatalytic Degradation of Organic Pollutants

Cited by 69 publications

References 51 publications

Polyoxometalate-based electron transfer modulation for efficient electrocatalytic carbon dioxide reduction

Polyoxometalate-based electron transfer modulation for efficient electrocatalytic carbon dioxide reduction

A Sodalite‐Type Silver Orthophosphate Cluster in a Globular Silver Nanocluster

2D/2D heterostructured photocatalyst: Rational design for energy and environmental applications

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