Chenwei Lu, Benjamin Clayville, Ji Yong Choi et al. · Chem · 2023
To synthesise how two-dimensional conductive metal-organic frameworks are characterised and tuned electronically, focusing on band gaps, band positions, metal-linker orbital interactions, linker design and structural perturbations.
The review’s argument is preserved as a navigable set of section summaries.
Defines c-MOF band structure in extended-solid terms and compares theoretical tools with UV-vis/Tauc, diffuse reflectance, UPS/LEIPS, CV and Mott-Schottky approaches.
Relevance: Core · p002 · Determining the electronic structure of conductive MOFs
Positions guest doping, charge-transfer complexes, oxidant uptake, metalation and conductive-polymer filling as ways to modulate conductivity, with the caveat that many examples are extrinsic rather than intrinsic conduction.
Relevance: Core · p008 · Host-guest interaction · Figure 3B
Treats interlayer spacing, alkyl side chains, exfoliation, pillar insertion and axial coordination as routes to manipulate out-of-plane coupling, band gap and conductivity.
Relevance: Core · p010 · Interlayer modulation · Figure 3C
Frames crystalline hybrid-organic materials and 2D c-MOFs as tunable alternatives to amorphous organic electronics, while stressing that most MOFs are electronically localised and poorly conductive.
Relevance: Core · p002 · Introduction
Reviews mixed-metal and mixed-linker frameworks as lattice-level routes to continuously tune band gaps, conductivity and band positions, while noting limited reported examples and crystallinity comparability issues.
Relevance: Core · p007 · Mixed component strategy · Figure 3A
Argues for rational selection of metal nodes and linkers based on orbital energy, symmetry, coordination geometry, functional groups and donor-acceptor concepts, together with relevant characterisation.
Relevance: Core · p011 · Outlook
Uses Table 1 and Figure 2 to compare calculated and experimental band gaps and conductivities, highlighting metal-node choice, coordinating elements and linker conjugation as design variables.
Relevance: Core · p005 · Reported electronic properties of 2D c-MOFs · Table 1
Classification systems are attributed to this review and are not treated as a global material registry.
The review distinguishes theoretical predictions from experimental observations and repeatedly treats mismatches as interpretive evidence about defects, finite crystallinity and characterisation limitations.
Categories: band structure and DOS calculations · experimental band gaps and band energies · defect and crystal-size mediated discrepancies
p003 · Theoretical methods
Figure 2 sorts linker motifs by primary coordinating atoms, pi-conjugated size/symmetry and additional functional groups such as alkyne pockets or alkyl side chains.
Categories: coordination elements · conjugation length · functional sites
p007 · Reported electronic properties of 2D c-MOFs · Figure 2
Figure 1 organises experimental methods by whether they estimate optical band gap, absolute band positions or electrochemical flat-band/redox-derived energies.
Categories: UV-vis/Tauc and Kubelka-Munk diffuse reflectance · UPS and LEIPS photoelectron spectroscopy · cyclic voltammetry · Mott-Schottky electrochemical impedance analysis
p004 · Experimental methods · Figure 1
The review's main synthetic-method framework groups tuning routes into compositional mixing, guest-mediated electronic perturbation and control of interlayer coupling.
Categories: mixed component strategy · host-guest interaction · interlayer modulation
p008 · Synthetic methods for tuning electronic structure of 2D conductive MOFs · Figure 3
Review-defined families retain their representative materials and conduction descriptions.
Copper 2D c-MOFs that compare O, N, S and Se coordinating elements across related linker motifs.
Conduction: Softer and more polarizable coordinating elements are interpreted as increasing covalency and metal-linker delocalisation; S/Se examples are described as metallic by UPS.
Representative materials: Cu-HHB · Cu-HAB · Cu-BHT · Cu-BHS
Nodes / linkers: Cu · hexahydroxybenzene · hexaaminobenzene · benzenehexathiol · benzenehexaselenol
p005 · Reported electronic properties of 2D c-MOFs
Alkyl side-chain functionalised HATI-based nickel 2D c-MOFs used to tune exfoliation, interlayer spacing and coupling.
Conduction: Longer alkyl chains expand interlayer spacing, reduce electronic coupling, increase band gap and suppress conductivity.
Representative materials: Ni3(HATI-C1)2 · Ni3(HATI-C3)2 · Ni3(HATI-C4)2
Nodes / linkers: Ni · hexaaminotriindole with alkyl side chains
p010 · Interlayer modulation
Hexahydroxytriphenylene/catecholate-linked frameworks including lanthanide and gallium variants used to discuss interlayer and pi-stacking transport.
Conduction: Used to discuss conductivity through pi-pi stacking and interlayer-distance effects, including out-of-plane metallic dispersion in Ln-HHTP.
Representative materials: Ln-HHTP · Ga-HHTP · Zn-HHTP
Nodes / linkers: lanthanides · Ga · Zn · hexahydroxytriphenylene · catecholate
p010 · Interlayer modulation
Hexaiminotriphenylene-based 2D c-MOFs in which Co, Ni and Cu nodes tune the electronic structure and conductivity.
Conduction: Review-framed as a platform where metal substitution or alloying can alter band gap, free-carrier concentration, activation energy and electrical conductivity.
Representative materials: Cu-HITP · Ni-HITP · Co-HITP · mixed MM'-HITP alloys
Nodes / linkers: Co · Ni · Cu · hexaiminotriphenylene
p007 · Mixed component strategy
BTC-based MOFs used as host lattices where dopants or metal substitution alter band structure and conductivity.
Conduction: Used to illustrate conductivity imparted or tuned through guest coordination, charge-transfer complexes and mixed-metal electronic states.
Representative materials: Cu3(BTC)2 · TCNQ@Cu3(BTC)2 · Co-substituted Cu3(BTC)2
Nodes / linkers: Cu · Co · benzene-1,3,5-tricarboxylate
p009 · Host-guest interaction
2D conductive MOFs built from macrocyclic linkers with internal alkyne pockets that host metal ions.
Conduction: The review interprets metalation as enabling intervalence charge transfer between inserted metal species and the 2D c-MOF host.
Representative materials: Ni2+ metalated macrocyclic-linker 2D c-MOF · Co2+ metalated macrocyclic-linker 2D c-MOF
Nodes / linkers: Cu · Ni guest ions · Co guest ions · macrocyclic alkyne-pocket linker
p009 · Host-guest interaction
A mixed-linker copper framework series combining HAB and TATHB to tune N/O coordinating-element ratios in the crystal lattice.
Conduction: Increasing HAB/N content is reported to continuously adjust band structure and raise conductivity over orders of magnitude.
Representative materials: Cu-TATHB · Cu-(TATHB)(HAB) · Cu3(HAB)x(TATHB)2-x
Nodes / linkers: Cu · hexaaminobenzene · triaminotrihydroxybenzene
p008 · Mixed component strategy
Review-level synthesis principles remain separate from primary-study recipes.
Coordinate small molecules such as water or urea at unsaturated metal nodes to reorganise stacking and charge transport.
Claimed effects: Substitution of water with bulkier urea in Zn-HHTP is reported to reorganise stacking distance and change conductivity ten-fold.
Controlling variables: axial molecule size · coordination at unsaturated metal nodes · stacking distance
Representative materials: Zn-HHTP
Caveat: The review presents this as an extension of post-synthetic coordination rather than a mature general method.
p011 · Interlayer modulation
Introduce electron acceptors, oxidants or conductive guests into MOF pores to create charge-transfer interactions, redox hopping or guest-derived conductive pathways.
Claimed effects: TCNQ, TCNE, iodine and conducting polymers are presented as conductivity-enhancing guests, with effects ranging from orders of magnitude to billion-fold changes.
Controlling variables: guest identity · guest loading · coordination to open metal sites · host pore accessibility
Representative materials: TCNQ@Cu3(BTC)2 · TCNE@Zn2TTFTB · iodine-doped pillar-layered MOF · polypyrrole-filled Cd MOF
Caveat: The review explicitly warns that most large-guest examples exhibit extrinsic rather than intrinsic conductivity.
p009 · Host-guest interaction
Build alkyne-pocket macrocycles into a conductive MOF so inserted metal ions perturb the host by intervalence charge transfer.
Claimed effects: The review reports increased conductivity after metalation and frames the result as functionality imparted through linker architecture.
Controlling variables: macrocyclic pocket design · inserted metal ion identity · metal-alkyne interaction strength
Representative materials: Ni2+ and Co2+ metalated macrocyclic-linker 2D c-MOF
Caveat: Presented as a specialised example rather than a broad, established family.
p009 · Host-guest interaction · Figure 2C
Vary linker ratios within a 2D c-MOF lattice to tune primary coordinating elements and band energies without discovering an entirely new framework family.
Claimed effects: The review reports continuous adjustment of band structure and a three-order conductivity increase as nitrogen content rises in Cu3(HAB)x(TATHB)2-x.
Controlling variables: HAB:TATHB ratio · nitrogen/oxygen coordinating element ratio · linker energy matching · lattice compatibility
Representative materials: Cu3(HAB)x(TATHB)2-x
Caveat: Only few mixed-linker c-MOFs are reported, leaving room for broader exploration.
p008 · Mixed component strategy
Blend multiple metal nodes within one framework to shift orbital energies, free-carrier concentrations and band positions while retaining an isostructural lattice.
Claimed effects: Continuous tuning of band gap, electrical conductivity and charge-transport activation energy is reported for HITP alloys; Co incorporation in Cu3(BTC)2 reduces the calculated band gap.
Controlling variables: metal identity · metal ratio · compatibility of metal geometry and linker symmetry · crystallinity comparability
Representative materials: MM'-HITP · Co-substituted Cu3(BTC)2
Caveat: The review stresses that few mixed c-MOF structures have been reported and crystallinity differences complicate comparisons.
p007 · Mixed component strategy
Insert pillaring ligands into layered conductive MOFs to alter interlayer distance and metal-node orbital interactions.
Claimed effects: Computationally, pillar pi-acceptor character is predicted to control bonding across layers; experimentally, bpy insertion in Cu3(THQ)2 reduces conductivity by disrupting out-of-plane overlap.
Controlling variables: pillar ligand identity · pi-accepting character · sigma donor character · interlayer distance
Representative materials: Ni3(HAB)2 with DABCO/bpy/pyz pillars · bpy-inserted Cu3(THQ)2
Caveat: Pillarisation may lower bulk conductivity even when it offers controlled structural modification.
p011 · Interlayer modulation
Use side-chain functionalisation to expand interlayer spacing and modulate exfoliation and stacked-layer coupling.
Claimed effects: Increasing side-chain length in Ni3(HATI-Cn)2 expands spacing, increases band gap, reduces carrier mobility and suppresses conductivity.
Controlling variables: alkyl side-chain length · interlayer spacing · degree of exfoliation · stacking-induced coupling
Representative materials: Ni3(HATI-Cn)2
Caveat: The review notes that practical control and mechanistic understanding of interlayer spacing effects are still incomplete.
p010 · Interlayer modulation
These are the review authors’ synthesis, not newly measured results.
2D c-MOFs are framed as a tunable class of crystalline electronic materials whose chemical and electronic modularity could support next-generation hybrid electronics.
Evidence basis: review_reasoning
Caveat: Applications are described as relatively underexplored.
p001 · Summary
For c-MOFs, the review recommends treating the material as an extended solid where metal-node and linker orbitals mix into continuous bands.
Evidence basis: single_reference
Caveat: This is an interpretive model; experimental disorder can complicate the idealised band picture.
p002 · Determining the electronic structure of conductive MOFs
Host-guest approaches can strongly enhance conductivity, but the review cautions that many large-guest examples primarily create extrinsic rather than intrinsic conductivity.
Evidence basis: multi_reference
Caveat: This distinction is essential when using these values in a transport chapter.
p009 · Host-guest interaction
For layered c-MOFs, increasing interlayer spacing generally weakens interlayer electronic coupling, increases band gaps and lowers out-of-plane conductivity.
Evidence basis: multi_reference
Caveat: The review states that practical methods and mechanistic insight are not yet fully developed.
p010 · Interlayer modulation
The review repeatedly identifies limited organic linker diversity as a bottleneck for fine-tuning c-MOF electronic structures.
Evidence basis: review_reasoning
Caveat: This is a field-level assessment rather than a quantitative count of linker space.
p006 · Reported electronic properties of 2D c-MOFs
Mixed metal and mixed linker systems are presented as lattice-level strategies for tuning electronic structure without abandoning established c-MOF platforms.
Evidence basis: multi_reference
Caveat: The review notes that few mixed-component c-MOFs are available.
p007 · Mixed component strategy
Most MOFs have limited or negligible electrical conductivity because their framework electronic structures are inherently localised.
Evidence basis: multi_reference
Caveat: 2D c-MOFs are treated as an important exception and opportunity.
p001 · Introduction
The review argues that complementary experimental measurements are needed because calculations and single characterisation tools can misrepresent c-MOF band structures.
Evidence basis: multi_reference
Caveat: Ni3HITP2 is used as an example where metallic calculations and experimental band gap observations diverge.
p003 · Theoretical methods
Optical band gaps should be distinguished from electronic band gaps: optical measurements generate excitonic transitions and are often only an approximation to electronic gaps.
Evidence basis: multi_reference
Caveat: The review notes that approximation is more justified when exciton binding energies are low.
p002 · Determining the electronic structure of conductive MOFs
The outlook recommends matching metal-node energy/symmetry and linker frontier orbitals, with linker functionalisation and donor-acceptor design as future routes to small-gap c-MOFs.
Evidence basis: review_reasoning
Caveat: The donor-acceptor argument is extrapolated partly from organic semiconductor design.
p011 · Outlook
Changing coordinating elements from O/N toward softer S/Se is interpreted as increasing covalency, delocalisation and metallic character in related Cu 2D c-MOFs.
Evidence basis: multi_reference
Caveat: Increased node density may also contribute to conductivity, so coordinating element softness is not the sole possible cause.
p005 · Reported electronic properties of 2D c-MOFs
Across reported 2D c-MOF properties, the review identifies a general trend that experimental band gaps exceed calculated values, attributed to defects and limited crystal size.
Evidence basis: multi_reference
Caveat: The statement is review-level synthesis from Table 1 rather than a controlled meta-analysis.
p005 · Reported electronic properties of 2D c-MOFs · Table 1
Every row remains visibly secondary and links to a primary dossier only where the mapping is verified.
| Material | Property | Reported value | Context and quality | Primary evidence | Review source |
|---|---|---|---|---|---|
| Secondarybpy-inserted Cu3(THQ)2 | electrical conductivity change | ~10^-8 to ~10^-10 S/cm | Post-synthetic bpy pillarisation in Cu3(THQ)2. Text · Approximate | research_0038 | p011 · Interlayer modulation |
| SecondaryTCNQ@Cu3(BTC)2 | electrical conductivity | 0.07 S/cm | Review text; TCNQ guest forms charge-transfer complex in Cu3(BTC)2. Text · Exact Reported | research_0088 | p009 · Host-guest interaction |
| SecondaryCo-substituted Cu3(BTC)2 | electrical conductivity change | 2.0 x 10^-10 to 1.4 x 10^-8 S/cm | Introduction of Co2+ into Cu3(BTC)2 host framework. Text · Range | No verified corpus mapping | p008 · Mixed component strategy |
| SecondaryCu-BHS | electrical conductivity | 110 S/cm | Review text summarising reported Cu-BHS conductivity; measurement details not extracted here. Text · Exact Reported | No verified corpus mapping | p003 · Theoretical methods |
| SecondaryCu-BHT | electrical conductivity | 1,580 S/cm | Four-contact probe according to Table 1 footnote. Table · Exact Reported | research_0006 | p006 · Reported electronic properties of 2D c-MOFs · Table 1 |
| SecondaryCu-HHB | optical band gap | 0.95 eV | Table 1 lists optical band gap unless marked as electronic; no asterisk is printed for this value. Table · Exact Reported | No verified corpus mapping | p006 · Reported electronic properties of 2D c-MOFs · Table 1 |
| SecondaryCu-HHB | electrical conductivity | 1.2 x 10^-6 S/cm | Two-contact probe according to Table 1 footnote. Table · Exact Reported | No verified corpus mapping | p006 · Reported electronic properties of 2D c-MOFs · Table 1 |
| SecondaryCu-(TATHB)(HAB) | electrical conductivity | 2.0 x 10^-6 S/cm | Four-contact probe according to Table 1 footnote. Table · Exact Reported | research_0441 | p006 · Reported electronic properties of 2D c-MOFs · Table 1 |
| SecondaryNi3(HATI-Cn)2 | calculated band gap change | 0.09 to 0.23 eV | Exfoliation and increased alkyl side-chain length from methyl to butyl groups. Text · Range | research_0056 | p010 · Interlayer modulation |
| SecondaryNi3(HATI-Cn)2 | electrical conductivity change | ~10^-2 to ~10^-4 S/cm | Exfoliation and optical band-gap increase after alkyl side-chain modulation. Text · Approximate | research_0056 | p010 · Interlayer modulation |
| SecondaryLn-HHTP | electrical conductivity | 9.0 x 10^-5-5.0 x 10^-2 S/cm | Two-contact probe according to Table 1 footnote; range across lanthanide variants. Table · Range | research_0047 | p006 · Reported electronic properties of 2D c-MOFs · Table 1 |
| Secondarypolypyrrole-filled [Cd(NDC)0.5(PCA)] | conductivity enhancement factor | 1 billion-fold | Polypyrrole incorporated into MOF void space via in situ polymerisation. Text · Rounded Reported | No verified corpus mapping | p010 · Host-guest interaction |
Open questions are presented as review-author priorities, not conclusions from the primary database.
Applications of 2D c-MOFs in electronic devices remain relatively underexplored despite their conductivity and tunability.
Proposed direction: Use electronically tunable 2D c-MOFs in accessible, application-directed device studies after band-energy and transport characterisation.
p001 · Summary
Defects, finite crystal size and characterisation limits complicate the correlation of calculated band structures with experimental band gaps.
Proposed direction: Pair calculations with multiple experimental probes such as UPS/LEIPS, UV-vis, CV and Mott-Schottky measurements.
p003 · Theoretical methods
Practical control of interlayer stacking distance and mechanistic understanding of its electronic consequences remain incomplete.
Proposed direction: Systematically vary side chains, pillars, axial ligands and metal-node spacing while measuring band dispersion, mobility and conductivity.
p010 · Interlayer modulation
The current c-MOF library is constrained by a small set of organic linkers and compatible metal-node symmetries.
Proposed direction: Expand planar pi-conjugated linker designs and functionalised linker motifs informed by orbital energies and symmetry matching.
p006 · Reported electronic properties of 2D c-MOFs
Synthetic methodologies are not yet sufficiently diverse to realise fine tunability of 2D c-MOF electronic structure.
Proposed direction: Develop mixed-component, host-guest and interlayer-modulation methods on well-studied c-MOF platforms.
p002 · Introduction
Few mixed-component c-MOF structures and few synthetic approaches are available, limiting compositional fine tuning.
Proposed direction: Develop mixed-metal and mixed-linker systems with comparable crystallinity and explicit electronic-property correlations.
p007 · Mixed component strategy
Mappings show which printed review references have a verified counterpart in the frozen primary corpus.
| Reference | Study | Role and context | Corpus mapping |
|---|---|---|---|
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