Chemical Scissor-mediated Structural Editing of Inorganic Materials

doi:10.15541/jim20230527

Abstract

Abstract:

Inspired by gene scissor concept in biological genetic engineering, chemical scissors, as important research tools, play an important role in the study of structure editing and application of materials. We aim to review the research progress of chemical scissors in structural editing and applications of materials. First of all, we introduce the basic concept and mechanism. Chemical scissors strategy refers to a methodology for material editing through which the main crystal structure is preserved but targeted atoms or structural units are knocked out, replaced, repaired or reconstructed in order to realize special functionality. Subsequently, the specific applications of chemical scissors in materials structure editing are discussed in depth, including the methods and functional designs for precise structure modulation of materials by chemical shearing, modification, synthesis, as well as etching and intercalation. Finally, the future research direction of chemical scissors in the field of material structure editing is envisioned, including developing new chemical scissors that are more intelligent and efficient, exploring more innovative strategies for material structure editing, understanding the underlying chemical mechanism, and further expanding the applicability of chemical scissors. Overall, we summarize the research progress and potential of material structural editing, which provides important theoretical and experimental support for further exploring and developing the application of chemical scissors in the field of materials.

Key words: chemical scissor, inorganic material, structural editing, perspective

CLC Number:

TB383

DING Haoming, CHEN Ke, LI Mian, LI Youbing, CHAI Zhifang, HUANG Qing. Chemical Scissor-mediated Structural Editing of Inorganic Materials[J]. Journal of Inorganic Materials, 2024, 39(2): 115-128.

Figures/Tables 16

Table 1 Chemical mechanism of typical "chemical scissors" and applications in structural editing

Regulation mechanism	Chemical scissor	Chemical mechanism	Target	Potential applications	Ref.
Chemical cutting	Plasma	Collision and reaction of plasma on graphene surface	Graphene	Electronic engineering	[13, 16]
	O₂/NH₃	Oxidation of edge carbon atoms	Graphene	Electronic engineering	[17]
	Metal nanoparticles	Catalytic hydrogenation of carbon atoms	Graphene	Electronic engineering	[18-19]
	TiO₂ photocatalysis	Photoinduced oxidation of carbon atoms by highly active OH radicals	Graphene	Electronic engineering	[12]
	HNO₃/H₂SO₄/KClO₃	Thermal expansion caused by oxidation and decomposition of surface functional groups of graphite	Graphite	Energy storage	[20]
	NH₃/H₂O₂	Oxidation of carbon atoms	g-C₃N₄	Catalysis, Sensor	[21]
	HNO₃/H₂SO₄	Oxidation of carbon atoms	g-C₃N₄	Catalysis, Sensor	[22]
Chemical modification	FeCl₃	Oxidation of Pd atoms	Pd clusters	Catalysis, Sensor	[23]
	H₂	Hydrogenation of N atoms	g-C₃N₄	Catalysis, Sensor	[24]
	CO₂	Oxidation of carbon atoms	Carbon materials	Energy storage	[25]
Chemical synthesis	C₂H₅OH	The breaking of organic bonds results in the dissolution of organic substances	3-aminophenol formaldehyde resin	Catalysis	[14]
	Acetone	The breaking of organic bonds results in the dissolution of organic substances	3-aminophenol formaldehyde resin	Catalysis, energy storage	[26-27]
	Lone pair cations and halogen ions	Control of coordination environments	Sb₂ZnO₃Cl₂ Sb₁₆Cd₈O₂₅Cl₁₄ Te₆O₁₁Cl₂ Sb₄O₅Cl₂	Catalysis, energy storage	[15, 28-29]
	H⁺	Control of reaction dynamics	Metal-benzene hexethiol (BHT) coordination polymer	Catalysis	[30]
Chemical etching and intercalation	Lewis acidic melts (CuCl₂, ZnCl₂)	Oxidation of A-site atoms in MAX phases	MAX phases	Catalysis, energy storage, electronic engineering	[10, 31-35]
	HF, HCl/LiF	Acidic dissolution of A-site atoms in MAX phases	MAX phases	Catalysis, energy storage	[36-37]
	Metal atoms (Mn, Fe, Co, Ni,Cu, Ag)	Regulating electronic structure by injecting electrons into host materials	Transition metal chalcogenides	Catalysis, energy storage	[38]

Table 1 Chemical mechanism of typical "chemical scissors" and applications in structural editing

Regulation mechanism	Chemical scissor	Chemical mechanism	Target	Potential applications	Ref.
Chemical cutting	Plasma	Collision and reaction of plasma on graphene surface	Graphene	Electronic engineering	[13, 16]
	O₂/NH₃	Oxidation of edge carbon atoms	Graphene	Electronic engineering	[17]
	Metal nanoparticles	Catalytic hydrogenation of carbon atoms	Graphene	Electronic engineering	[18-19]
	TiO₂ photocatalysis	Photoinduced oxidation of carbon atoms by highly active OH radicals	Graphene	Electronic engineering	[12]
	HNO₃/H₂SO₄/KClO₃	Thermal expansion caused by oxidation and decomposition of surface functional groups of graphite	Graphite	Energy storage	[20]
	NH₃/H₂O₂	Oxidation of carbon atoms	g-C₃N₄	Catalysis, Sensor	[21]
	HNO₃/H₂SO₄	Oxidation of carbon atoms	g-C₃N₄	Catalysis, Sensor	[22]
Chemical modification	FeCl₃	Oxidation of Pd atoms	Pd clusters	Catalysis, Sensor	[23]
	H₂	Hydrogenation of N atoms	g-C₃N₄	Catalysis, Sensor	[24]
	CO₂	Oxidation of carbon atoms	Carbon materials	Energy storage	[25]
Chemical synthesis	C₂H₅OH	The breaking of organic bonds results in the dissolution of organic substances	3-aminophenol formaldehyde resin	Catalysis	[14]
	Acetone	The breaking of organic bonds results in the dissolution of organic substances	3-aminophenol formaldehyde resin	Catalysis, energy storage	[26-27]
	Lone pair cations and halogen ions	Control of coordination environments	Sb₂ZnO₃Cl₂ Sb₁₆Cd₈O₂₅Cl₁₄ Te₆O₁₁Cl₂ Sb₄O₅Cl₂	Catalysis, energy storage	[15, 28-29]
	H⁺	Control of reaction dynamics	Metal-benzene hexethiol (BHT) coordination polymer	Catalysis	[30]
Chemical etching and intercalation	Lewis acidic melts (CuCl₂, ZnCl₂)	Oxidation of A-site atoms in MAX phases	MAX phases	Catalysis, energy storage, electronic engineering	[10, 31-35]
	HF, HCl/LiF	Acidic dissolution of A-site atoms in MAX phases	MAX phases	Catalysis, energy storage	[36-37]
	Metal atoms (Mn, Fe, Co, Ni,Cu, Ag)	Regulating electronic structure by injecting electrons into host materials	Transition metal chalcogenides	Catalysis, energy storage	[38]

Fig. 1 Preparation of graphene nanoribbons by photolithographic plasma etching technique[13] (a, b) Schematic illustrations of preparation of graphene nanoribbons by photolithographic plasma etching technique; (c, d) Atomic force microscope (AFM) images of graphene nanoribbons prepared by photolithographic plasma etching technique; AFM images of graphene nanoribbons, showing morphologies before (e) and after (f) cutting using NH3/O2 as chemical scissor

Fig. 2 Metal nanoparticles as catalyst scissors cutting graphene [19] (a) Schematic illustration of the cutting process of graphene using metal nanoparticles as catalyst scissors; (b) Schematic illustration of the cutting pathway of graphene; (c-e) AFM images of graphene after cutting, showing the cutting pathway

Fig. 3 Photocatalytic cutting of graphene[12] (a) Schematic illustration of the photocatalytic approach to engineering single or few-layer graphene, in which the quartz plate/TiO2 thin film/ patterned Cr photomask is put into contact with graphene; (b) Optical microscope image of graphene ribbons obtained with a line-shape TiO2 photomask; (c) SEM image of a photo-catalytically patterned CVD-graphene with inset showing the photomask structure; (d) Optical microscope image of a patterned reduced graphene oxide (RGO) film, illustrating the feasibility of complex structural design; (e) SEM image of a periodically patterned RGO film; (f) SEM image of a series of CVD-graphene ribbons having different widths. Scale bars: 50 μm (b-e), 100 μm (inset in (c)), 10 μm (f)

Fig. 4 Schematic illustration of scanning probe microscopy (SPM) technique for cutting graphene nanosheets[11]

Fig. 5 H2SO4/HNO3 as chemical scissors cutting g-C3N4 [22] (a) Schematic illustration of cutting g-C3N4 using H2SO4/HNO3 as chemical scissors; (b-f) TEM images of samples with different mixed acid volume ratios (V(HNO3)∶V(H2SO4)= (b) 1∶3, (c) 1∶2, (d) 1∶1, (e) 2∶1, (f) 3∶1)

Fig. 6 Pd single-atom modification by selectively trimming the Pd atoms on the PCN surface using chemical scissors[23] (a-d) Schematic illustration of Pd single-atom modification by selectively trimming the Pd atoms on the PCN surface using chemical scissors; (e-h) Chemical mechanism and reaction process of Pd single-atom modification by selectively trimming the Pd atoms on the PCN surface using chemical scissors

Fig. 7 N atomic vacancy modification of g-C3N4 realized by cutting of H2 chemical scissor[24] (a) Schematic illustration of N atomic vacancy modification of g-C3N4 realized by cutting of H2 chemical scissor; (b-d) Band structures of g-C3N4 before and after modification

Fig. 8 Mg/Zn/CO2 scissors rationally tailoring the carbon nanomaterials[25] (a, b) Molecular scissors acting on the surface of carbon nanomaterials; (c, d) Highly interconnected microstructure of tubular superstructure of nanocarbon (TSNC) facilitating substantial ion-reserved accommodation and rapid mass-transfer expressway; (e-j) TEM images of the obtained carbon nanomaterials, showing different cutting morphologies

Fig. 9 Preparation of hollow nanostructure using chemical scissors (a) Schematic illustration and reaction mechanism of modulation of nanostructure and chemical composition by using ethanol as chemical scissors to precisely cut formaldehyde resin[26]; (b-e) Illustrations of the deflation-inflation asymmetric growth (DIAG) process and mechanism[27]

Fig. 10 Schematic representation of structural conversion using dppm as chemical scissor[60]

Fig. 11 Two-dimensional MOF materials synthesized by proton concentration modulation with chemical scissor effect[30] (a) Chemical reaction mechanism of Cu-BHT; (b) Interfacial self-assembly growth process, and (c) schematic illustration of metal vacancy engineering via precise pH regulation (yellow sphere: proton; black sphere: C atom; gold sphere: S atom; green sphere: Cu atom; red circle: Cu vacancy)

Fig. 12 Schematic illustrations of different etching methods for preparation of MXene (a) HF as echant[36]; (b) KF-NaF-LiF melt as echant[68]

Fig. 13 Chemical-scissors assisted structural editing strategy for layered transition metal carbides/nitrides[10] (a) Schematic illustration of chemical-scissors assisted structural editing strategy for layered transition metal carbides/nitrides; (b) Periodic table showing elements involved in the formation of MAX phases and MXenes. Light blue: M elements; brown: A elements; black: X elements; green: ligand (T) elements; circled: elements studied in the present work

Fig. 14 Lewis-acidic-melt method for the preparation of MAX phases and MXenes (a) Schematic illustration of preparing novel MAX phases and MXene based on Lewis-acidic-molten-salt route[31]; (b) STEM image of Ti3C2Cl2 prepared by Lewis-acidic-molten-salt route, and its corresponding atomic model[31]; (c) Schematic illustration of preparing Ti3C2Tx MXene via a reaction between Ti3SiC2 and CuCl2; (d) Redox potential/Gibbs free energy between Lewis acid cations and A-site atoms in molten salts[34]

Fig. 15 Chemical scissor-assisted atomic intercalation of transition metal dichalcogenides[38] (a) Intercalation schematic of Cu-TiS2 in LiCl-KCl eutectic molten salt at 360 ℃; (b-d) FFT patterns of pristine TiS2 diffraction spots, Cu0.125TiS2, and Cu0.5TiS2 diffraction superspots taken along the [0001] zone-axis direction; (e, f) Ti2p and Cu2p XPS analysis of CuxTiS2 (x=0, 0.125, and 0.5); (g) Raman analysis of CuxTiS2 (x=0, 0.05, 0.125, 0.25, and 0.5)

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