Surface Atom Rearrangement and Electron Delocalization of the Sub-nanometric Materials★

doi:10.6023/A23050214

Acta Chimica Sinica ›› 2023, Vol. 81 ›› Issue (10): 1462-1470.DOI: 10.6023/A23050214 Previous Articles

Special Issue: 庆祝《化学学报》创刊90周年合辑

Review

亚纳米尺度材料表面原子重排与电子离域^★

张东政, 刘清达, 王训^*()

清华大学化学系稀土新材料教育部工程研究中心北京 100084

投稿日期:2023-05-08 发布日期:2023-07-05

作者简介:

张东政, 2018年获得中国科学技术大学化学学士学位, 目前为清华大学化学系博士研究生, 师从王训教授. 主要研究方向为亚纳米线凝胶的设计、合成和应用.

王训, 清华大学化学系教授, 博士生导师. 2004年于清华大学化学系获得博士学位, 2007年任清华大学化学系教授, 同年获得国家杰出青年科学基金, 2014年获得教育部“长江学者”特聘教授称号, 主要致力于无机纳米晶体新结构控制合成、形成机制及组装, 已在Science, Nature, Nat. Chem., Nat. Synth., Sci. Adv., Nat. Commun.等SCI期刊上发表文章三百余篇, 兼任《化学学报》、《中国科学: 化学》、《高等学校化学学报》、《结构化学》、《无机化学学报》编委, Editorial board member of Advanced Materials, Editorial board member of Nano Research, Scientific Editor of Materials Horizons, Associate Editor of Science China Materials, Associate Editor of Science Bulletin, Associate Editor of Nano Research, 中国化学会副秘书长.

^★庆祝《化学学报》创刊90周年.

基金资助:
国家自然科学基金(2224100031)

Surface Atom Rearrangement and Electron Delocalization of the Sub-nanometric Materials^★

Dongzheng Zhang, Qingda Liu, Xun Wang()

Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing 100084

Received:2023-05-08 Published:2023-07-05
Contact: *E-mail: wangxun@mail.tsinghua.edu.cn
About author:
^★Dedicated to the 90th anniversary of Acta Chimica Sinica.
Supported by:
National Natural Science Foundation of China(2224100031)

Subnanometer scale is an important feature size in the field of material science. Sub-nanometric materials (SNMs) have several unique properties different from molecular-based or traditional nanomaterials, and their size is comparable to the diameters of the polymer single strand/DNA, clusters and the single unit cell of inorganic crystals. The surface atom ratio of SNMs is close to 100%, which brings significant surface atom rearrangement and electron delocalization effects. 1D SNMs are expected to become an entry point to break the boundary between polymers and inorganic materials due to their excellent structural flexibility, machinability, viscosity and gelation. Electron delocalization in SNMs changes the electronic and band structures of the materials, and significantly enhances the external field coupling effects, resulting in excellent photothermal conversion and catalysis properties. This review focuses on the surface atom rearrangement and electron delocalization effects at the subnanometer scale. The precise synthesis and assembly, polymer-like properties, electronic structure, and catalytic properties of SNMs are introduced. It is hoped that this review can help to deeply understand the coupling law of subnanometer scale interactions and structure-function relationship, further promoting the accurate synthesis of SNMs and the construction of functional systems.

Key words: sub-nanometric material, polymer-like property, catalysis, electron delocalization, surface atom rearrangement

Cite this article

Dongzheng Zhang, Qingda Liu, Xun Wang. Surface Atom Rearrangement and Electron Delocalization of the Sub-nanometric Materials^★[J]. Acta Chimica Sinica, 2023, 81(10): 1462-1470.

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Fig. & Tab. 10

Figure 1. Flexibility and adjustability of subnanostructures (a) GdOOH subnanowires (SNWs); (b) Ca-polyoxometalate (POM) SNWs; (c) indium sulfide subnanobelts (SNBs); (d) 2D superstructures self-assembled from indium sulfide SNBs; (e) polyoxometalate single clusters SNWs; (f) polyoxometalate single clusters subnanorings. Reproduced with permission from ref. [15], copyright 2013 American Chemical Society; ref. [16], copyright 2022 The Authors; ref. [17], copyright 2013 American Chemical Society; ref. [18], copyright 2019 The Authors.

Figure 2. GdOOH SNWs chiral assemblies (a) Spiral SNWs bundles; (b) macroscopic helical assemblies; (c) local structure of macroscopic helical assemblies; (d) circular dichroism spectrum (CD) spectra of macroscopic helical assemblies; (e) CD spectra of macroscopic helical assemblies with addition of organic dyes; (f) molecular dynamics simulation of the chiral evolution. Reproduced with permission from ref. [19], copyright 2020 American Chemical Society.

Figure 3. Ca-POM SNWs adhesive (a) Adhesive performance of SNWs; (b~e) adhesive performance for different substrates, times, temperatures and cycles; (f) underwater adhesive performance. Reproduced with permission from ref. [20], copyright 2022 American Chemical Society.

Figure 4. SNWs organogels (a) GdOOH SNWs; (b) (CTA)3(TBA)3P2W18O62 SNWs; (c) Fe3O4-PMo12, Bi2O3-PMo12, Bi2O3-PMo12/S and Bi2O3-PMo12/V SNWs; (d) self-supporting organogels formed by Ca-POM SNWs with Dundahl effect; (e) use of Ca-POM SNWs to recover gasoline; (f~h) elasticity and flexibility of Ca-POM SNWs organogels. Reproduced with permission from ref. [15], copyright 2013 American Chemical Society; ref. [16], copyright 2022 The Authors; ref. [21], copyright 2013 The Authors; ref. [22], copyright 2021 Wiley-VCH.

Figure 5. SNWs macroscopic films (a) Electrospun fibers of GdOOH SNWs; (b) a single SNWs fiber; (c) large-area macroassembly mat; (d) preparation process of wet spinning and (e~g) the resulting GdOOH SNWs film; (h) anisotropic scattering of visible light in GdOOH SNWs films; (i, j) polarization fluorescence properties of SNWs films composited with quantum dots; (k) hydroxyapatite SNWs-polyimide films with high transparency and haze; (l) composite gel coatings used for different transparent substrates. Reproduced with permission from ref. [23], copyright 2017 American Chemical Society; ref. [24], copyright 2019 Wiley-VCH; ref. [25], copyright 2022 Wiley-VCH.

Figure 6. A novel 2D sub-nanometric material system-clusterphene (a, b) Structure characterization of single layer clusterphene; (c) structural representation of clusterphene (Nd, pink; W, gold; O, red; H, white); (d) molecular orbital interactions and electron delocalization of clusters; (e) the adiabatic ionization energy of POM clusters in different oxidation states; (f) the differential charge density of clusterphene (Cu, cyan; Nb, light blue; O, red; H, white; N, dark blue; C, gray); (g) the charge changes in electron population with one electron loss in clusterphene; (h) the partial density of states of clusterphene (the Fermi level was set as 0?eV as shown by dashed lines). Reproduced with permission from ref. [30], copyright 2022 The Authors; ref. [32], copyright 2023 The Authors.

Figure 7. Fullerene covalent network (a, b) Monolayer quasi-hexagonal phase C60; (c, d) few-layer quasi-tetragonal phase C60; (e) electronic band structure of the monolayer quasi-hexagonal phase C60 nanosheets; (f) angle-resolved Raman spectrum of monolayer quasi-hexagonal phase C60; (g) the conductivities of a monolayer quasi-hexagonal phase C60 device; (h) optical micrograph of a Mg4C60 single crystal; (i) photoluminescence spectra of molecular C60, bulk graphullerite and bilayer graphullerene; (j) thermal conductivities of a graphullerite flake and a C60 single crystal at room temperature. Reproduced with permission from ref. [35], copyright 2023 The Authors; ref. [36], copyright 2022 The Authors

催化剂	底物	反应时间/min	反应温度/℃	砜化率/%	转化速率/(mmol•g^－1•h^－1)	稳定性
ZrO₂-[PMo₁₂O₄₀]^3－ SNBs	DPS	25	25	100	14.4	5次循环后保持100%
	MPS	25	25	100	14.4
	DBT	30	50	78	9.36
TiO₂-[PMo₁₂O₄₀]^3－ SNBs	DPS	10	25	100	36.0	5次循环后保持100%
	MPS	10	25	100	36.0
	DBT	15	50	100	24.0
ZnO-Zn(OH)₂-Mo₆O₁₉亚纳米片(SNSs)	THT	3	20	100	170.1
	MPS	3	20	100	127.2
	DPS	2	20	100	134.4
	DBT	50	20	100	4.9
ZnO-Zn(OH)₂-Mo₈O₂₆ SNSs	THT	2	20	100	255.2
	MPS	2	20	100	190.8
	DPS	1	20	100	268.9
	DBT	25	20	100	9.8
ZnO-PMo₁₂O₄₀ SNSs	THT	2	20	100	255.2	6次循环后保持100%
	MPS	2	20	100	190.8
	DPS	3	20	100	89.6
	DBT	50	20	100	4.9

Table 1. Catalytic activity of thioether oxidation in subnanometer binary heterostructures

Figure 8. Subnanometer heterostructures used for photoelectrocatalysis and photothermal conversion (a) Monolayer 2D porphyrin-metal organic framework(MOF) structure and (b) its performance in photoelectrocatalytic reduction of CO2 to C2 products; (c) structure of Au-PW12 SNWs and (d) their performance in photoelectrocatalytic reduction of CO2 to CO; (e) structure of metal phthalocyanine-polyoxo- metalate sandwich nanosheets and (f) their performance in photoelectrocatalytic reduction of CO2 to CO; (g) morphology of CuO-PMA SNSs; (h) heating curves and (i) photothermal images of CuO-PMA SNSs dispersions at different time points under irradiation. Reproduced with permission from ref. [40], copyright 2022 Wiley-VCH; ref. [41], copyright 2021 American Chemical Society; ref. [42], copyright 2020 Wiley-VCH; ref. [43], copyright 2019 American Chemical Society.

Figure 9. Subnanometer alloys used for the electrocatalytic hydrogen oxidation reaction (a, b) Morphology characterizations of RhMo SNSs; (c) the schematic atom model of RhMo SNSs (Rh, white; Mo, purple); (d) mass and specific activities of RhMo SNSs/C, Rh/C, and Pt/C; (e) the morphology characterization of high-entropy alloys (HEA) SNWs; (f) normalized mass activity and specific activity at an overpotential of 50 mV versus reversible hydrogen electrode; (g) 3D models and the enlarged atomic model of HEA SNWs. Reproduced with permission from ref. [44], copyright 2023 The Authors; ref. [46], copyright 2023 The Authors.

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亚纳米尺度材料表面原子重排与电子离域^★

Surface Atom Rearrangement and Electron Delocalization of the Sub-nanometric Materials^★

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亚纳米尺度材料表面原子重排与电子离域★

Surface Atom Rearrangement and Electron Delocalization of the Sub-nanometric Materials★

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亚纳米尺度材料表面原子重排与电子离域^★

Surface Atom Rearrangement and Electron Delocalization of the Sub-nanometric Materials^★