Surface chemistry of MXene quantum dots: Virus mechanism-inspired mini-lab for catalysis

doi:10.1016/S1872-2067(22)64167-6

Chinese Journal of Catalysis ›› 2022, Vol. 43 ›› Issue (11): 2913-2935.DOI: 10.1016/S1872-2067(22)64167-6

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Surface chemistry of MXene quantum dots: Virus mechanism-inspired mini-lab for catalysis

Yuhua Liu, Wei Zhang^*(), Weitao Zheng^#()

Key Laboratory of Automobile Materials MOE, and School of Materials Science & Engineering, and Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials, and Electron Microscopy Center, and International Center of Future Science, Jilin University, Changchun 130012, Jilin, China

Received:2022-06-21 Accepted:2022-08-16 Online:2022-11-18 Published:2022-10-20
Contact: Wei Zhang, Weitao Zheng
About author:Wei Zhang (Jilin University) obtained his Ph.D. degree at the Institute of Metal Research Chinese Academy of Sciences in 2004. Then He held positions in NIMS-Japan, Samsung AIT-South Korea, Fritz-Haber Institute of MPG-Germany, DTU-Denmark and CIC Energigune-Spain. He was awarded Ikerbasque Research Professor in 2016. In 2014, he became a full professor at Jilin University and has been selected as Tang Auchin Scholar Leading Professor since 2020; Now he serves as the Director of the Electron Microscopy Center of Jilin University. His current research focuses on surface and interface of advanced energy materials and catalysts. Prof. Zhang was invited as a member of the editorial board of Communications Chemistry at Nature Publishing Group.
Weitao Zheng (Jilin University) is Cheung Kong Distinguished Professor and Vice President of Jilin University. He obtained his Ph.D. degree at Jilin University in 1990. After that, he held positions at the Royal Institute of Sweden, Linköping University, Chiba Institute of Technology, and Nanyang University of Technology. His current research focuses on energy materials, functional thin films, and catalysts. Prof. Zheng was invited as an editorial board member of Applied Surface Science and Vacuum.
Supported by:
National Natural Science Foundation of China(51872115);National Natural Science Foundation of China(51932003);2020 International Cooperation Project of the Department of Science and Technology of Jilin Province(20200801001GH)

Abstract

Abstract:

Scientific research is currently more interdisciplinary. Researchers have parsed the surface structure of virus, constructed the interaction model of virus-receptors, offering the clues for studying efficient targeted drugs. Likewise, catalysis is also highly relevant to modern human life. Exploring the surface structure and physicochemical properties of catalysts is of great significance for the design of efficient catalysts. Great progresses have been made for endowing specific physicochemical properties of catalysts through controlling the size of materials and coordination chemistry of active sites, particularly at nanometer scale since Sir John Meurig Thomas and Tao Zhang’s early ground-breaking contribution, with casting on a very surface issue. Herein, functional regulation renders the emerging MXene quantum dots (MQDs) excel in contrast to the typical carbon-based quantum dots. In fact, similar to the interaction of virus-receptors model, the surface functional groups decorated MQDs provide a mini-lab to afford a variety of adjustments, involved with the type modification and electronic structure tuning of groups as well as their arrangement, together with the interaction between the groups and active materials/support, ultimately for packaging or designing high-activity catalysts.

Key words: Surface chemistry, Functional group, Structure characterization, Mxene, Quantum dot

Yuhua Liu, Wei Zhang, Weitao Zheng. Surface chemistry of MXene quantum dots: Virus mechanism-inspired mini-lab for catalysis[J]. Chinese Journal of Catalysis, 2022, 43(11): 2913-2935.

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Figures/Tables 21

Fig. 1. (a,b) Comparison of the structures between carbon materials quantum dots and MQDs. (c) Functional groups of MQDs for specific functionalization. (d) The structure of novel coronavirus SARS-CoV-2. Reprinted with permission from Ref. [22]. Copyright 2020, Nature Publishing Group.

Fig. 2. Modification of surface functional groups of MQDs at single site catalyst (SSC).

Fig. 3. (a) Schematic diagram of MXene and MQDs. (b) Comparison of HER overpotentials at current density of 10 mA cm-2 between different metal-based MXene and MQDs.

Fig. 4. (a) Mechanistic illustration of NRR and free energy on the Ti-edge of bare MXene, and F, OH position of Ti3C2F2, Ti3C2(OH)2. (b) NH3 yield for the different catalysts. Reprinted with permission from Ref. [47]. Copyright 2020, Wiley. (c) STEM image of Ti3C2 MQDs with defects. (d) Charge density difference of Ti3C2 MQDs. (e,f) Adsorption energy of O2, LiO2 molecules in optimized MQDs structure. (g-i) Charge density difference of Ti3C2 MQDs and adsorption energy of O2, LiO2 molecules. Reprinted with permission from Ref. [51]. Copyright 2021, Wiley. (j) Charge density difference of Ti2CTx MQDs/Cu2O heterogenous structure. (k) Functional groups evolution. Reprinted with permission from Ref. [52]. Copyright 2022, Wiley.

Fig. 5. (a) Energy band structure of 2D MXene and 0D MQDs. (b) Photocatalytic mechanism diagram of MQDs.

Fig. 6. Design of heterogeneous structure between semiconductor photocatalyst and MQDs. (a) Ti3C2 MQDs as electrons donors in Ti3C2-QD/Ni-MOF heterojunctions. Reprinted with permission from Ref. [57]. Copyright 2020, ACS. (b) Ti3C2 MQDs as electrons acceptors in Ti3C2-QDs/ZnIn2S4/Ti Flower-like heterojunction. Reprinted with permission from Ref. [58]. Copyright 2020, MDPI. (c) Z-Scheme heterostructure of BiVO4@ZnIn2S4/Ti3C2 MQDs composites. Reprinted with permission from Ref. [60]. Copyright 2020, Elsevier. (d-f) S-Scheme heterostructure of TiO2/C3N4/Ti3C2 MQDs composites. Reprinted with permission from Ref. [59]. Copyright 2020, Elsevier. (g) Photoelectrocatalytic mechanism of Co-MQDs. Reprinted with permission from Ref. [61]. Copyright 2020, Wiley. (h) Photoelectrocatalytic mechanism of MQDs as reservoirs of HTL. Reprinted with permission from Ref. [62]. Copyright 2022, Wiley.

Table 1 The controllable synthesis and applications of MQDs.

MQDs	Type of groups	Synthesis	Catalytic applications	Ref.
Ti₃C₂T_x	-O, -OH, -F	Hydrothermal	Water oxidation	[62]
Ti₃C₂(OH)₂	-OH	Alkalization treatment	Electrocatalytic N₂ reduction	[47]
Ti₃C₂T_x	-O, -OH, -F, -Cl	Cell-crushing	Photocatalytic HER	[58]
Ti₂CT_x	-O, -OH, -Cl	Acid treatment	Electrocatalytic HER	[52]
Ti₃C₂T_x	-O, -OH, -F	hydrothermal	Photocatalytic N₂ photofixation	[74]
Ti₃C₂T_x	-O, -OH, -F, -Cl	Sonication	Electrocatalytic HER	[32]
V₂CT_x	-O, -OH, -F	Sonication	Electrocatalytic HER	[32]
Nb₂CT_x	-O, -OH, -F, -Cl	Sonication	Electrocatalytic HER	[32]
Ti₃C₂T_x	-O, -OH, -F, -Cl	Sonication	Photocatalytic Cr⁴⁺ reduction, BPA oxidation	[75]
Ti₃C₂T_x	-O, -OH, -F	Solvothermal	Li-O₂ Batteries	[51]
Ti₃C₂T_x	-O, -OH, -F, -NH₂	Sonication	Photocatalytic H₂O₂ production	[76]
Ti₃C₂T_x	-O, -OH, -F, -Cl	Sonication	Photocatalytic TC degradation	[77]
Ti₃C₂T_x	-O, -OH, -F	Hydrothermal	Zinc-air batteries	[78]
Ti₃C₂T_x	-O, -OH, -F	Reflux	Photocatalytic NO	[79]
Ti₃C₂T_x	-O, -OH, -F	Hydrothermal	Photocatalytic N₂ reduction	[57]
Ti₃C₂T_x	-O, -OH, -F	Hydrothermal	Photocatalytic CO₂ reduction	[59]
Ti₃C₂T_x	-O, -OH, -F	Hydrothermal	Photocatalytic water splitting	[60]
Ti₃C₂T_x	-O, -OH, -F	Hydrothermal	Electrocatalytic ORR, MOR	[80]
Ti₃C₂T_x	-O, -OH, -F	Hydrothermal	Photocatalytic HER	[81]
Ti₃C₂T_x	-O, -OH, -F	Hydrothermal	Photocatalytic CO₂ reduction	[55]

Fig. 7. Synthesis of Ti3C2Tx MQDs with -F, -OH, -O and -NH2 groups (a) and the FTIR spectra of Ti3C2Tx MQDs (c). Reprinted with permission from Ref. [64]. Copyright 2017, Wiley. Synthesis of Ti3C2Tx MQDs with -F, -OH, -O groups (b) and the FTIR spectra of Ti3C2Tx MQDs (d). Reprinted with permission from Ref. [58]. Copyright 2021, MDPI. Synthesis of Ti3C2Cl2 MQDs with -Cl groups (e) and the FTIR of Ti3C2Cl2 MQDs (f). Reprinted with permission from Ref. [72]. Copyright 2022, Elsevier. Synthesis of Ti3C2 MQDs with O-containing groups (g) and the XPS spectra of Ti3C2 MQDs (h). Reprinted with permission from Ref. [73]. Copyright 2017, RSC.

Fig. 8. (a) Schematic illustration of and HRTEM image of Ru@CDs. (b) Schematic illustration of and HRTEM image of Ru@PC. (c) Schematic illustration of and HRTEM image of Ru@P-AC. Reprinted with permission from Ref. [89]. Copyright 2020, RSC. (d) Overpotential summarization of Ru and different support, 5 wt% Ru/C catalysts based on Ref. [89]. (e) HRTEM images of N-CDs@Co. Inset: Schematic illustration of N-CDs@Co. Reprinted with permission from Ref. [93]. Copyright 2019, ACS. (f) Overpotential summarization of different CD-based catalysts-based Ref. [93] in 0.5 mol L?1 H2SO4, 1 mol L?1 KOH, respectively.

Fig. 9. (a) HAADF-STEM image of Ti3C2 MQDs with edge defects and grain boundary. (b) HAADF-STEM of Ti3C2 MXene nanosheets (MNS). (c) EPR spectra of MQDs/N-C, MNS/N-C and single MQDs/N-C. Reprinted with permission from Ref. [51]. Copyright 2021, Wiley-VCH. (d) Synthesis route of TinO2n-1 QDs with oxygen vacancies. (e) EPR spectra of OV-TinO2n-1 QDs@porous carbon nanosheets. (f) Adsorption energies of Li2S4 on the surface of TinO2n-1 QDs with and without OVs, inset Fig. is crystal structure of Ti3C5 QDs. Reprinted with permission from Ref. [98]. Copyright 2021, Wiley-VCH. (g) Mechanism of defect induced FL. (h) Time-dependent FL intensity of MQDs after adding Ni2+. Reprinted with permission from Ref. [101]. Copyright 2021, ACS.

Fig. 10. Total density of states (TDOS) and electronic band structures of Ti8C4O8 (a) and Ti8C4O6P2 (b). Local density of states (LDOS) of Ti8C4O8 (c) and Ti8C4O6P2 (d). (e) Schematic diagram of O 2p orbital orientation vary from O 2px to O 2pz after P doping; Dissociation barrier of H2O and release barrier of H of Ti8C4O8 (f) and Ti8C4O6P2 (g). Reprinted with permission from Ref. [27]. Copyright 2018, Wiley. (h) Mechanistic illustration of hybrid orbital between H and O in V2CO2. (i) Mechanism of hybrid orbital between H and O in V2CO2 after introducing metal atom. (j-l) Difference charge density of V2CO2 after introducing transition metal under the same Ni coverage of 12.5 ML%. (m) Difference charge density of V2CO2 with 16.7 ML% coverage. (n) Gibbs free energy of H adsorption ΔGH at T0 sites (12.5% ML) as a function of strain. Reprinted with permission from Ref. [28]. Copyright 2016, Wiley.

Fig. 11. (a) TEM image of LDH/MQDs. (b) Geometric structure model of LDH/MQD composite. (c) HRTEM image of LDH/MQDs. (d) LSV curves of different catalysts for ORR and OER. Reprinted with permission from Ref. [78]. Copyright 2021, Wiley. (e) TEM image of MoS2 QDs @Ti3C2MQDs @MWCNTs. (f,g) LSV curves of different catalysts for ORR and MOR. Reprinted with permission from Ref. [80]. Copyright 2019, Elsevier. (h) Structural schematics of Ti2C MQDs/Cu2O/Cu foam electrocatalyst. (i) LSV curves of Ti2C MQDs/Cu2O/Cu foam for HER reaction. Reprinted with permission from Ref. [52]. Copyright 2022, Wiley.

Fig. 12. (a) Self-crosslinked mechanism of graphene QDs. (b) Morphology of self-crosslinked process; TEM image of GQDs-NH2 and SEM images of freeze-dried Ir/GQDs-NH2. Reprinted with permission from Ref. [87]. Copyright 2021, Springer. (c) TEM image of Ru@CQDs, inset: size distribution of the Ru particle. (d) TEM image of Ru@CQDs. (e) LSV curves of different Ru-based catalysts. Reprinted with permission from Ref. [112]. Copyright 2018, Wiley. (f) Model of Pt nanoparticles. (g) Terraces population of (100), (111), and step sites of Pt nanoparticles as a function of Pt particle sizes. Reprinted with permission from Ref. [113]. Copyright 2022, ACS. (h-j) Computational model of bare M2C, Ti2CO2 and Mo2CO2 MXene. Reprinted with permission from Ref. [29]. Copyright 2020, Elsevier.

Fig. 13. (a) Atomic force microscope (AFM) image of Ti2CTx MXene nanosheets. (b) Structure models of Ti2CTx with the different amount fluorine atoms. (c) LSV curves of Ti2CTx before and after removing -F groups. Reprinted with permission from Ref. [43]. Copyright 2018, Elsevier. (d) Volcano curves of exchange current (i0) as a function of the average Gibbs free energy (ΔGaH*). Reprinted with permission from Ref. [108]. Copyright 2017, ACS. (e) Bader charge of V3CNO2-2x(OH)2x at different -OH coverage. (f) Gibbs free energy of hydrogen adsorption on the surface of M3CNO2-2x(OH)2x at different -OH coverage. Reprinted with permission from Ref. [117]. Copyright 2017, Elsevier. (g) Partial density of states (PDOS) of Ti2CT2 with different functional groups. Reprinted with permission from Ref. [119]. Copyright 2013, APS. (h) Gibbs free energy calculation of Ti3C2 MQDs with different functional groups. Reprinted with permission from Ref. [47]. Copyright 2020, Wiley.

Fig. 14. (a) TEM image of Ti3C2 MQDs/Cu nanocomposite. (Inset: Inverse Fourier Transform of interface between MQDs and Cu). (b) DOS of Cu side, MQDs side and MQDs/Cu. (c) Charge density difference of MQDs/Cu. (d) NH3 yield of Cu, MQDs and MQDs/Cu electrocatalyst. Reprinted with permission from Ref. [120]. Copyright 2022, Wiley. (e,f) TEM images of WO3/TQDs. (g,h) TEM images of WO3/TQDs/In2S3. (i) UV-vis diffuse reflectance spectroscopy of different catalysts. (j) Photocatalytic activity of different catalysts. (k) Schematic illustration of WO3/TQDs/In2S3. Reprinted with permission from Ref. [75]. Copyright 2021, Elsevier.

Fig. 15. Summarizing the characterization techniques of surface functional groups. Reprinted with permission from Ref. [47,72,101,107,124]. Copyright 2020, Wiley & Copyright 2021, ACS & Copyright 2021, Wiley & Copyright 2021, Elsevier & Copyright 2021, Elsevier, respectively.

Fig. 16. (a) Atomic-resolution HAADF images of Cl-terminated layered Ti3C2 MXene. Insets: the enlarged views of the atomic positions correspond to crystal structure of the right, and the atomic-scale EDS maps. Reprinted with permission from Ref. [125]. Copyright 2021, Springer Nature. (b) HAADF image of Ti3C2Br2 MXene sheets. (c) Line scan profile of elemental analysis. Reprinted with permission from Ref. [126]. Copyright 2020, AAAS. (d) HAADF-STEM image of Ti3C2 MQDs clusters. (e) HAADF-STEM and TEM images of single Ti3C2 MQDs. Reprinted with permission from Ref. [51]. Copyright 2021, Wiley.

Fig. 17. In-situ/operando characterization technique of CF-O and CF-FeSO catalysts. (a) In-situ/operando Raman spectroscopy electrochemical cell. (b) Raman spectroscopy of CF-O. (c) Raman spectroscopy of CF-FeSO. (d) In-situ/operando NEXAFS electrochemical cell. (e) Co-K edge XANES spectrum. (f) Co L-edge NEXAFS spectrum. Reprinted with permission from Ref. [130]. Copyright 2022, Springer Nature.

Fig. 18. (a) Morphology of β-CoOOH particles at different voltage (Scale bars: 500 nm). (b) Variation of CoO layers with the change of voltage. (c) Line scan of nanoparticles height (top) and the relationship of height-voltage (bottom). (d) Operando STXM equipment. (e) STXM-XAS spectra of Co LIII-edge. (f) Steady-state voltage-dependent phase images of β-Co(OH)2 nanoparticles. Scale bar, 1 μm. Reprinted with permission from Ref. [131]. Copyright 2021, Springer Nature. (g) In-situ APXPS equipment. (h) APXPS spectra of Co2p3/2. Reprinted with permission from Ref. [132]. Copyright 2017, ACS. (i) Operando XRD patterns of the NiCeOxHy catalyst under different potentials. Reprinted with permission from Ref. [133]. Copyright 2018, Nature Publishing Group.

Fig. 19. Energy band structure of Ti2C MXene (a), Ti2CO2 (b), and Ti2C(OH)2 (c). (d) Surface Pourbaix diagrams of Ti2C. (e) Stability of Ti2C with different O* and OH* species. Reprinted with permission from Ref. [108]. Copyright 2016, ACS. (f) Interface structure model of Cr2CO2. (g) Gibbs free energy of Cr2CO2 at different H coverage. Reprinted with permission from Ref. [137]. Copyright 2019, ACS. (h-j) Structure models of NC, MoC, and MoC@NC. (k) HER free energy diagram of NC, MoC, and MoC@NC. Reprinted with permission from Ref. [138]. Copyright 2022, Wiley-VCH. (l) HER activation energy calculation of catalysts. Reprinted with permission from Ref. [139]. Copyright 2018, Springer Nature.

Fig. 20. The challenges of MQDs.

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Surface chemistry of MXene quantum dots: Virus mechanism-inspired mini-lab for catalysis

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