Chapter Four · failure evidence

What Porous Materials & MOFs got wrong, from 40 dissertations

The compiled records demonstrate various operational and synthetic failure points across porous materials and metal-organic frameworks. Performance limitations frequently arise from structural collapse under moisture or acidic gas exposure, pore obstruction from chemical functionalization, and competition against simpler commercial benchmark adsorbents. These records come from PhD theses at 19 institutions, 2021 to 2026. Each links to its thesis. They were extracted by language models reading the full text, so treat each as a lead to read, not a verdict.

Novel porous adsorbents perform worse than commercial or simpler baseline materials

9 theses · 8 institutions

Synthesized porous materials, biochars, and metal-organic frameworks achieved lower adsorption capacities for gases, heavy metals, and organic contaminants than commercial activated carbons and zeolites. These custom adsorbents also exhibited slower conversion rates and reduced pollutant removal efficiencies compared to established benchmark materials.

Lost to a baseline

Mesoporous carbon spheres synthesized by Chen et al. (2021) achieved 3.22 mmol/g CO2 capture capacity at 75 °C and 0.05 bar, outperforming MC2-800-1-60 (2.95 mmol/g at 0.15 bar).

Development of Three-Dimensional Mesoporous Biocarbon Materials for Energy-Related Applications · University of Nottingham Repository

Lost to a baseline

Carboxylic CNT/CoFe2O4 composite achieved 250 mg/g SMX adsorption capacity, outperforming this work.

ADSORPTION OF PHARMACEUTICALS FROM CONTAMINATED WATER BY ADSORBENTS DEVELOPED FROM REED CANARY GRASS · HARVEST

Lost to a baseline

PEI-modified mesoporous carbon spheres (MCSs) by Wang et al. (2016) achieved 3.71 mmol/g CO2 capture capacity at 75 °C and 15% CO2, higher than MC2-800-1-60 (2.95 mmol/g).

Development of Three-Dimensional Mesoporous Biocarbon Materials for Energy-Related Applications · University of Nottingham Repository

Lost to a baseline

Activated carbon prepared from coal baseline achieved a higher maximum SMX adsorption capacity (264.4 mg/g) than this work's renewable adsorbent (147.9–161.3 mg/g).

ADSORPTION OF PHARMACEUTICALS FROM CONTAMINATED WATER BY ADSORBENTS DEVELOPED FROM REED CANARY GRASS · HARVEST

Lost to a baseline

Commercial activated carbon (AC) achieved 94% PFOA adsorption efficiency, outperforming PBC (92%) and ZnBC (84%) under identical batch conditions (200 µg/L PFOA, 10 h, 25 °C)

REMOVAL OF PERFLUOROALKYL SUBSTANCES (PFAS) FROM WATER USING MODIFIED BIOCHAR ADSORBENTS PRODUCED FROM CANOLA STRAW · HARVEST

Lost to a baseline

F300 commercial activated carbon achieved higher maximum Langmuir PFOS adsorption capacity (55.7 mg/g) than SCGKOH biochar (43.4 mg/g)

Development of Novel Biochar-Molecularly Imprinted Polymer Composites for Targeted Adsorption of Per- and Polyfluoroalkyl Substances in Water Treatment Applications · ResearchWorks

Lost to a baseline

Zn-EDTA MOF CO2 adsorption capacity (164.58 ml/g) was beaten by Mg-MOF-74 (593.0 ml/g)

تحضير جسيمات أكسيد الزنك النانونية وهياكل عضوية معدنية لتقليل الانبعاثات الكربونية ومعالجة المياه · DSpace at University of El Oued

Lost to a baseline

Activated carbon (20,200 µg/g) and activated alumina (15,900 µg/g) exhibited far higher As(V) adsorption capacities than IOCB (836.4 µg/g).

Removal of arsenic from drinking water by fungal biomass and biological filtration. · oURspace

Lost to a baseline

Polyurethane sponge-supported graphene oxide-titanium phosphate achieved 228.1 mg/g and phosphorus-functionalized nanoporous carbon achieved 347.0 mg/g Dy3+ adsorption capacity, beating PCs/MB (34.0 mg/g).

Development of a novel and green Mannich reaction-modified chitosan hydrogel for dysprosium(III) recovery · Iowa State

Lost to a baseline

Fe3O4-FITC-resin MB adsorption capacity (150 mg g-1) was lower than covalent organic frameworks (~300 mg g-1), reduced graphene oxide (~200 mg g-1), and metal-organic frameworks (~180 mg g-1).

Scalable Synthesis of Nanomaterials in Continuous-Flow Reactors · Georgia Tech

Lost to a baseline

At 250 °C for 1 h with 1 wt.% ethanol, impregnated 2 wt.% Ru/CeO2 showed ~20% lower H2 productivity than commercial 5 wt.% Ru/Al2O3 (443 vs. 554 mmol H2/gRu) and lower ethanol conversion (1.3 vs. 1.7 mol/gRu) primarily due to ~21% lower surface area and microporous structure.

Valorisation of biomass-derived wastewaters via aqueous phase reforming for energy recovery: a multi-level performance assessment · IRIS - POLITO - prod

Chemical functionalization and post-synthetic modifications reduce pore volume and adsorption uptake

8 theses · 5 institutions

Functionalizing organic linkers or carbon surfaces with amines, metal ions, or counterions often reduced available pore volume and blocked gas diffusion channels. Consequently, modified sorbents showed lower gas adsorption capacities and poorer cyclic stability than unmodified framework baselines.

Tried and failed

Post-synthetic metalation of functionalised porous frameworks applied to gas adsorption selectivity. Outcome: worse than baseline. Reason: Metal coordination reduced available adsorption sites and pore volume compared to unmetalated framework

Metal-Organic Framework Structure-Property Relationships for Selective Sulfur Dioxide Adsorption · Georgia Tech

Tried and failed

post-synthetic amine functionalization for cyclic gas adsorption applied to metal-organic frameworks in dynamic breakthrough. Outcome: unstable. Reason: significant loss of adsorption capacity over repeated adsorption-desorption cycling compared to carbon and zeolites

Influence Of Water Vapor on the Adsorption of Exhaled Breath-Borne VOC Biomarkers for COVID-19 · Georgia Tech

Tried and failed

amine functionalization for low-concentration gas capture applied to porous materials for direct air capture. Outcome: worse than baseline. Reason: most amine-functionalized candidates failed performance screening criteria despite standard expectations for carbon dioxide capture

Accurate Predictions of the Adsorption Space and Efficient Sorbent Discovery in Metal-Organic Frameworks · Georgia Tech

Lost to a baseline

Non-functionalized activated carbon outperformed G2CO3-impregnated AC (10p, 15p, 20p) in pure CO2 adsorption at pressures above 45 kPa (5.044 mmol/g for AC vs 3.699-4.607 mmol/g).

Evaluating the Effect of Composition, Structure and Functionality on Atmospheric CO2 Adsorption in Porous Solid Sorbents · Virginia Tech

Lost to a baseline

Neat MIL-101-Cr-4 and MIL-101-Cr-10 outperformed their EN-functionalized counterparts in pure CO2 adsorption (7.09 vs 6.1 mmol/g and 7.35 vs 1.65 mmol/g).

Evaluating the Effect of Composition, Structure and Functionality on Atmospheric CO2 Adsorption in Porous Solid Sorbents · Virginia Tech

Tried and failed

gas-phase halogenation of porous framework linkers applied to small-pore metal-organic frameworks. Reason: small pore apertures restricted mass transport, causing pore blockage, incomplete reaction, and framework degradation

CONTROLLING TOXIC GAS CAPTURE AND DELIVERY IN METAL–ORGANIC FRAMEWORKS: FROM CHLORINE TO HYDROGEN SULFIDE · Cornell

Tried and failed

amine functionalization of organic linkers applied to low-pressure hydrogen adsorption in metal-organic frameworks. Outcome: worse than baseline. Reason: functional groups reduced pore volume and surface area without introducing sufficiently strong binding sites for hydrogen

Mixture Adsorption in Metal-Organic Frameworks for Biogas and Light Hydrocarbon Separation · Georgia Tech

Tried and failed

room-temperature synthesis of ionic metal-organic frameworks applied to porous materials for gas adsorption. Reason: extraframework counterions completely obstructed internal pore channels and structural voids to gas molecules

Neutral and ionic Co(II) metal-organic frameworks with 2-methylimidazole and trimesate: design and evaluation for molecule encapsulation and slow release. · Cambridge

Tried and failed

incorporating hydrophilic functional groups into porous frameworks applied to metal-organic framework water sorption. Outcome: worse than baseline. Reason: more hydrophilic substituents failed to lower the condensation relative humidity threshold compared to larger halides

Sorption-based atmospheric water harvesting: from atoms to applications · MIT

Exposure to water and humid cycling triggers hydrolytic degradation and framework collapse

4 theses · 3 institutions

Metal-organic frameworks and porous coordination frameworks suffered irreversible structural collapse and loss of surface area during repeated water adsorption cycles or steam exposure. Extended ambient humidity exposure also degraded porosity and severely reduced carbon dioxide uptake in direct air capture applications.

Tried and failed

post-synthetic hydroxide exchange applied to metal-organic frameworks for water sorption. Outcome: unstable. Reason: framework lost structural stability upon repeated water adsorption and desorption cycles

Tailoring Metal–Organic Frameworks for Water Harvesting · MIT

Tried and failed

rapid thermal dehydration in humid atmosphere applied to metal-organic frameworks for adsorption. Outcome: unstable. Reason: framework collapsed forming metal oxide domains within minutes instead of generating coordinatively unsaturated sites

MOFs beyond the framework: Investigating the role of polymeric guests, linker functionality, and structural disorder to enhance adsorption performance · EPFL

Tried and failed

solvothermal synthesis using dimethylformamide solvent applied to porous coordination frameworks. Outcome: unstable. Reason: residual solvent or defective coordination caused rapid hydrolytic degradation and structural collapse during water cycling

Tailoring Metal–Organic Frameworks for Water Harvesting · MIT

Tried and failed

water vapor adsorption beyond isotherm threshold applied to microporous coordination framework adsorbent. Outcome: unstable. Reason: moisture exposure caused irreversible structural collapse, severely reducing surface area and pore volume

Addressing the data gap in adsorption materials for direct air capture - an investigation of physicochemical, equilibrium sorption, and kinetic sorption properties · Imperial

Tried and failed

zinc-based metal-organic frameworks for cyclic adsorption applied to atmospheric water harvesting. Outcome: unstable. Reason: poor hydrolytic stability causing rapid loss of sorption capacity and surface area upon water cycling

Tailoring Metal–Organic Frameworks for Water Harvesting · MIT

Tried and failed

direct air capture using fluorinated MOFs applied to low-concentration CO2 adsorption in humid air. Outcome: unstable. Reason: extended exposure to humidity and ambient conditions causes severe loss of porosity and CO2 uptake capacity

Addressing the data gap in adsorption materials for direct air capture - an investigation of physicochemical, equilibrium sorption, and kinetic sorption properties · Imperial

Considered and rejected

Considered and rejected: rejected hydrotalcites and base metal oxides as water sorbents due to loss of steam adsorption capacity at methanol synthesis operating temperatures

Enhancing CO2 hydrogenation to methanol in fixed and fluidized bed reactors by selective in-situ adsorption of water · EPFL

High mass loading and intraparticle mass transfer resistances degrade porous electrode performance

5 theses · 5 institutions

Excessive electrodeposition loading on porous carbon electrodes increased electrical resistance and triggered active material dissolution during cycling. In addition, intraparticle mass transport limitations and mechanical deformation compromised catalyst selectivity and electrode stability.

Tried and failed

carbon nanotube immobilised molecular catalysts without stirring applied to photochemical carbon dioxide reduction. Outcome: worse than baseline. Reason: mass transport limitations in porous nanotube sheets under high flux reduced product selectivity

Organic Semiconductor-BiVO4 Tandem Devices for Solar-Driven H2O and CO2 Splitting. · Cambridge

Lost to a baseline

Cu-Mg-Al MMO-11 exhibited slower oxygen release and re-oxidation rates than the more porous Cu-Mg-Al MMO-9.5 due to higher intraparticle mass transfer resistances

Layered double hydroxide-derived oxygen carriers for chemical looping processes · Imperial

Tried and failed

prolonged electrodeposition of metal oxide applied to porous carbon supercapacitor electrodes. Outcome: worse than baseline. Reason: excessive active material loading increased electrical resistance, reducing specific capacitance at high scan rates

Electrochemical studies of the applications of novel carbon-based materials · Oxford

Tried and failed

block copolymer electrospun porous carbon fibers applied to flexible supercapacitor electrodes. Outcome: unstable. Reason: severe mechanical deformation caused structural degradation and contact loss in gel electrolyte

Block Copolymer Derived Porous Carbon Fiber for Energy and Environmental Science · Virginia Tech

Tried and failed

high mass loading of electrodeposited metal oxide applied to porous carbon supercapacitor electrodes. Outcome: unstable. Reason: active material dissolution and structural degradation during cycling

Electrochemical studies of the applications of novel carbon-based materials · Oxford

Lost to a baseline

Low-frequency capacitance of LIG potassium ISEs (~48-51 µF in water) was substantially lower than colloid-imprinted mesoporous (CIM) carbon contacts and carbon black nanocomposites (<1 µV/h drift).

Development and characterization of ion-selective electrodes based on laser-induced graphene for food safety and precision agriculture · Iowa State

Exposure to acidic gases or thermal activation causes framework degradation and collapse

5 theses · 4 institutions

Acidic gases like sulfur dioxide and hydrogen sulfide attacked coordination frameworks, causing metal sulfide formation, loss of crystallinity, and structural failure. In addition, heating during degassing activation caused flexible or weakened frameworks to buckle and lose their internal pore volume.

Tried and failed

gas capture using metal-organic frameworks applied to hydrogen sulfide adsorption. Outcome: unstable. Reason: framework degradation and loss of porosity occurred due to metal sulfide formation

CONTROLLING TOXIC GAS CAPTURE AND DELIVERY IN METAL–ORGANIC FRAMEWORKS: FROM CHLORINE TO HYDROGEN SULFIDE · Cornell

Tried and failed

thermal activation degassing applied to metal-organic framework gas sorption. Outcome: unstable. Reason: the porous framework collapsed upon heating during the degassing process

Silicon-based hexacarboxylic acids and their application in metal-organic frameworks · Imperial

Tried and failed

post-synthetic metal coordination of functionalized porous frameworks applied to acidic gas adsorption. Outcome: unstable. Reason: Metal coordination weakened framework stability, leading to structural collapse upon sulfur dioxide exposure.

Metal-Organic Framework Structure-Property Relationships for Selective Sulfur Dioxide Adsorption · Georgia Tech

Tried and failed

ligand functionalization with nitrogen heterocycles applied to metal-organic framework gas adsorption. Outcome: unstable. Reason: exposure to acidic gas caused framework collapse, severe loss of crystallinity, and porosity degradation

Tuning metal-organic frameworks for flue gas desulfurization · Georgia Tech

Tried and failed

incorporating flexible heterocyclic linkers in metal-organic frameworks applied to porous coordination framework synthesis. Outcome: unstable. Reason: framework collapsed and buckled upon activation due to excessive ligand flexibility, resulting in loss of porosity

Development of metal-organic frameworks based on N-heterocyclic ligands · EPFL

Harsh synthetic conditions and metalation cause undesired phases and metal nanoparticle aggregation

5 theses · 5 institutions

Elevated temperatures and altered synthesis parameters induced precursor reduction, nanoparticle aggregation, or the formation of unintended crystalline phases with low adsorption capacity. Mechanical processing like ball-milling and post-synthetic metal coordination also degraded crystal structures and caused unintended metal exchange at structural nodes.

Tried and failed

Post-synthetic metalation of Lewis-basic porous frameworks applied to phosphine-functionalized metal-organic frameworks. Outcome: unstable. Reason: Crystal degradation, desolvation, and unintended metal exchange at structural nodes prevented structural characterization.

Phosphine and arsine metal-organic frameworks for the heterogenization of 4d and 5d transition metal complexes · UT Austin

Tried and failed

increasing base concentration and antisolvent ratio in synthesis applied to continuous flow metal-organic framework synthesis. Reason: favored formation of an undesired crystalline phase with poor gas adsorption capacity

Magnetic framework composites for CO2 capture · University of Nottingham Repository

Tried and failed

ball-milling precursor mixture for porous film fabrication applied to fuel cell cathode catalyst layers. Outcome: worse than baseline. Reason: loss of macroporous structure during processing led to significantly reduced mass activity

Engineering the cathode catalyst layer architecture for fuel cells · Imperial

Tried and failed

High-temperature direct metallation of porous frameworks applied to metal-organic framework single-site metal loading. Outcome: unstable. Reason: Excess thermal energy caused precursor reduction and unwanted metal nanoparticle aggregation instead of single-site coordination

Supporting Well-Defined Platinum Group Metals in Metal-Organic Frameworks for Heterogeneous Catalysis · MIT

Considered and rejected

Considered and rejected: Rejected hard-template mesoporous synthesis due to low yields and requirement of hazardous etching reagents (NaOH, HF).

Scalable Synthesis of Nanomaterials in Continuous-Flow Reactors · Georgia Tech

Surface modifications on mesoporous nanoparticles cause burst release and erratic delivery kinetics

2 theses · 2 institutions

Polymer coatings on mesoporous nanoparticles triggered particle agglomeration and rapid burst release of cargo instead of controlled release. In vitro release measurements also failed to predict rapid in vivo clearance, while certain mesoporous oxide templates showed non-selective toxicity to healthy cells.

Tried and failed

polysaccharide surface coating for controlled release applied to mesoporous inorganic nanoparticles. Outcome: unstable. Reason: coating induced nanoparticle agglomeration and triggered non-selective burst release of loaded ions

Inorganic nanoparticles for cancer therapy · Imperial

Tried and failed

surface modification for sustained drug release applied to mesoporous biomaterial vaccine delivery systems. Outcome: did not generalise. Reason: in vitro release kinetics failed to predict in vivo rapid clearance indistinguishable from unmodified controls

Developing strategies to enhance immune responses induced by mesoporous silica rod vaccines · Harvard

Considered and rejected

Considered and rejected: Rejected GeO2 and GeO2-ZnO-SiO2 mesoporous nanoparticle templates due to poor dissolution, lack of selective cancer cytotoxicity, and unwanted toxicity to normal breast cells.

Inorganic nanoparticles for cancer therapy · Imperial

Left open by the authors

Problems the authors named and did not get to.

Left open

Test higher activation temperatures on N-doped mesoporous carbons to restore CO2 adsorption capacity after moist flue gas exposure. Blocker: Requires a materials synthesis and gas adsorption wet lab to treat materials and measure adsorption capacities.

Versatile, direct nanocasting strategy to N-rich ordered mesoporous carbons for selective post-combustion CO2 capture and energy storage · IRIS - POLITO - prod

Left open

Determine optimal desorption methods and measure the cycle life limits for VOC-loaded functionalized MOF and activated carbon adsorbent capsules. Blocker: Requires physical synthesis of MOFs, adsorption capsules, dynamic breakthrough gas chromatography apparatus, and wet lab facilities

Influence Of Water Vapor on the Adsorption of Exhaled Breath-Borne VOC Biomarkers for COVID-19 · Georgia Tech

Left open

Optimize the layering of functionalized MOF and activated carbon adsorbent beds for multicomponent dynamic breakthrough adsorption of breath-borne VOCs. Blocker: Requires experimental synthesis of functionalized MOFs and dynamic breakthrough gas chromatography testing apparatus under humid conditions.

Influence Of Water Vapor on the Adsorption of Exhaled Breath-Borne VOC Biomarkers for COVID-19 · Georgia Tech

Left open

Modify Zn-EDTA MOF structure and increase adsorbent dosage to evaluate and optimize CO2 capture efficiency and saturation limits. Blocker: Requires wet lab chemical synthesis and physical gas adsorption testing apparatus

تحضير جسيمات أكسيد الزنك النانونية وهياكل عضوية معدنية لتقليل الانبعاثات الكربونية ومعالجة المياه · DSpace at University of El Oued

Left open

Screen alternative MOF materials using the CO2 mass transfer and adsorption model to identify candidates with higher capacity or lower cost. Blocker: None

CARBON DIOXIDE ADSORPTION ON MOFS-COATED WIND TURBINE BLADES: MODELING AND FACTORS INFLUENCING ADSORPTION RATE · JScholarship

Left open

Synthesize and evaluate activated carbon-supported controls with various anions and guanidinium-carboxylic acid networks for CO2 adsorption. Blocker: Requires chemical synthesis lab and experimental breakthrough column testing apparatus.

Evaluating the Effect of Composition, Structure and Functionality on Atmospheric CO2 Adsorption in Porous Solid Sorbents · Virginia Tech

Left open

Evaluate dynamic breakthrough adsorption behavior of low-concentration (<= 10 ppm) VOC biomarkers on functionalized MOFs and activated carbons. Blocker: Requires wet lab synthesis of functionalized MOFs and dynamic breakthrough gas chromatography testing apparatus.

Influence Of Water Vapor on the Adsorption of Exhaled Breath-Borne VOC Biomarkers for COVID-19 · Georgia Tech

Left open

Measure dynamic CO2 adsorption capacity on MIL-101(Cr) before and after saturation exposure to SO2/NO2 across various partial pressures. Blocker: Requires a wet chemistry laboratory, physical MOF synthesis/activation, and gas breakthrough measurement apparatus.

Stability and Adsorption Properties of Metal-Organic Frameworks for Acid Gases · Georgia Tech

Left open

Synthesize and mechanistically characterize mesoporous MgO sorbents promoted with different or mixed alkali metals (Li, Na, K, Rb) for CO2 capture. Blocker: Requires a wet chemistry laboratory, chemical precursors, and physical characterization instruments.

Investigation Of Catalytic Sorbents For Capture And Conversion Of CO2 To Methane · Georgia Tech

Left open

Conduct comprehensive field testing of activated carbon adsorption capacities for multiple pollutants and heavy metals beyond arsenic. Blocker: Requires physical synthesis of activated carbon material and wet-lab or field-testing water filtration setups.

Approaches to maximise the utilisation of residues from thermal conversion of oil palm waste. · Cranfield

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