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Computationally guided search for OSDAs to crystallise aluminosilicate STF and IFR in hydroxide media

Can synthesis-energy ranking, machine-learning classification and de novo design over more than 10,000 OSDAs find an organic structure-directing agent that crystallises aluminosilicate STF or IFR in hydroxide media?

Source: Lessons from Failed Attempts of Computationally Guided Synthesis of Aluminosilicate STF and IFR Zeolites in Hydroxide Media (doi:10.1021/acs.chemmater.5c01751). Path record: acs-zeolite-path.json. Headline outcome negative-not-achievable. Experimental synthesis using a shortlist of OSDAs predicted to favor STF or IFR, in addition to AEI or CHA, did not yield the expected aluminosilicate products, and instead, amorphous materials were obtained in most cases. our experiments did not result in AEI or CHA being synthesized (neither STF nor IFR), and hence in this sense our predictions from calculations must be considered a failure. All graphs · Back to the pilot

How to read these graphs

A discourse graph breaks a piece of research into typed one-sentence nodes and draws how they bear on one another. The grammar is that of Discourse Graphs (Chan and Akamatsu). Read each graph left to right: a question, the experiments that addressed it, the results they produced, and the hypothesis every result is drawn against.

QUE Question: What the work set out to answer.
HYP Hypothesis: The answer the authors expected. Every result earns one edge against it.
EXP Experiment: One attempt at the question: a trial arm, an assay, a survey, an analysis.
RES Result: One finding from an experiment, with where in the source it comes from.
ISS Issue: An open question or untried branch the work leaves for someone else.

addresses: An experiment addresses the question.
produces: An experiment produces a result.
supports: A positive result that backs the hypothesis.
opposes: A negative result that counts as evidence against the hypothesis, or a refutation of an earlier claim.
informs: A partial or mixed result that bears on the hypothesis without settling it.
consistent with: A negative or inconclusive result that does not count either way: no positive control passed, or there is no sensitivity or power statement, so the absence of an effect cannot be told from a measurement that failed.
relation: A thin dotted line: a link the source itself states between two experiments, such as one being derived from another.

A dashed box marks a result the rule above counts as uninformative, or an issue. In the drawing, click a node to jump to its text below.

The graph

Read left to right. The question (QUE) is addressed by 4 experiments (EXP), each of which produces results (RES), and each result bears on the hypothesis (HYP) with one of four edges. 4 support it, 3 oppose it, 5 inform it, and 4 are merely consistent with it because the informativeness rule would not count them as evidence either way. Click a node to jump to its full text below.

supports positive finding
opposes informative negative, or refutation
informs partial finding
consistent with inconclusive or uninformative: no positive control passed, or no sensitivity statement
thin grey a relation the record itself states between two attempts
dashed box a result the informativeness rule marks uninformative, or an issue

The grammar is that of Discourse Graphs (Chan and Akamatsu): QUE, HYP, EXP, RES and ISS nodes with supports, opposes and informs edges. Every node and edge is derived from fields already in the Negative-Results Record; the edge a finding earns is decided by its outcomeClass and informativeness. Issues (ISS) hang below the graph as a strip: the open questions and untried branches the path leaves for someone else to pick up.

Nodes

Question and hypothesis

QUE: Can synthesis-energy ranking, machine-learning classification and de novo design over more than 10,000 OSDAs find an organic structure-directing agent that crystallises aluminosilicate STF or IFR in hydroxide media?
HYP: Use synthesis-energy calculations, machine-learning classifiers and de novo design over more than 10,000 organic structure-directing agents to find OSDAs that would crystallise the aluminosilicate forms of the STF and IFR zeolites in hydroxide media, then test the shortlist hydrothermally.

Experiments (4 attempts)

Node	Attempt	Type	Headline	JSON
EXP	Hydrothermal synthesis targeting aluminosilicate IFR with QG001780m gives only amorphous solids Six gel compositions from pure silica to Si/Al 10, at 175 to 200 °C for 14 to 42 days, all gave amorphous solids. The OSDA degraded during synthesis.	`wet-lab`	`inconclusive-no-positive-control`	record
EXP	Hydrothermal synthesis targeting aluminosilicate IFR with QG001780m2 gives amorphous solids, MOR, ZSM-12 or dense phases Fourteen gel compositions with Si/Al 10 to 100, with or without Na+ or K+, at 150 to 175 °C for 7 to 21 days gave amorphous solids, mordenite, ZSM-12 (MTW, ranked 13th in the prediction) or dense phases; never IFR.	`wet-lab`	`inconclusive-no-positive-control`	record
EXP	Synthesis-energy, machine-learning and de novo screen of more than 10,000 OSDAs predicts CHA and AEI everywhere and shortlists three OSDAs whose predictions the syntheses refute No OSDA makes STF or IFR the most stable aluminosilicate phase; 13 STF and 5 IFR candidates have the target in the top three. For the three synthesised, the predicted CHA, AEI, STF or IFR never formed, which the authors call a failure of the predictions.	`computational`	`refuted`	record
EXP	Hydrothermal synthesis targeting aluminosilicate STF with the shortlisted spirocyclic OSDA gives only amorphous solids Eight gel compositions from pure silica to Si/Al 10, at 150 to 200 °C for 14 to 50 days, all gave amorphous solids. The OSDA was a mixture of stereoisomers and degraded during synthesis.	`wet-lab`	`inconclusive-no-positive-control`	record

Results (16 findings)

Node	Finding	Id	Outcome and informativeness	Edge	JSON
RES	Does N-benzyl-N,N,2-trimethylpropan-2-aminium hydroxide crystallise aluminosilicate IFR from an aluminosilicate gel in hydroxide media without inorganic cations? target: aluminosilicate IFR; syntheses yielding aluminosilicate IFR = 0 (n = 12)	`ifr-not-formed` in acs-zeolite-ifr-synthesis-qg001780m	`inconclusive-no-positive-control` uninformative no positive control; no negative control; no sensitivity or power statement	consistent-with HYP	record
RES	Did N-benzyl-N,N,2-trimethylpropan-2-aminium (QG001780m) survive the hydrothermal conditions intact? target: N-benzyl-N,N,2-trimethylpropan-2-aminium (QG001780m); OSDA degradation in the mother liquor = intact cation progressively lost after 29 and 40 days	`osda-degraded` in acs-zeolite-ifr-synthesis-qg001780m	`positive` not-applicable rule applies to negative and inconclusive findings only	supports HYP	record
RES	Does N-benzyl-N,N-dimethylpropan-2-aminium crystallise aluminosilicate IFR under SSZ-42-type (Na+) or MCM-58-type (K+) hydroxide conditions? target: aluminosilicate IFR; syntheses yielding aluminosilicate IFR = 0 (n = 14)	`ifr-not-formed` in acs-zeolite-ifr-synthesis-qg001780m2	`inconclusive-no-positive-control` uninformative no positive control; no negative control; no sensitivity or power statement	consistent-with HYP	record
RES	Did N-benzyl-N,N-dimethylpropan-2-aminium (QG001780m2) survive the hydrothermal conditions intact? target: N-benzyl-N,N-dimethylpropan-2-aminium (QG001780m2); OSDA degradation after 1 to 4 days in Na+ or K+ gels = about 3 percent	`osda-intact` in acs-zeolite-ifr-synthesis-qg001780m2	`positive` not-applicable rule applies to negative and inconclusive findings only	supports HYP	record
RES	For how many of the 78 OSDAs taken from OSDB (36 active for STF, 42 inactive-close) is aluminosilicate STF the lowest-synthesis-energy phase? target: aluminosilicate STF; OSDAs for which STF is the most stable phase by E_syn = 0 (n = 78)	`esyn-landscape` in acs-zeolite-osda-screen	`positive` not-applicable rule applies to negative and inconclusive findings only	supports HYP	record
RES	Which screened or designed OSDAs place aluminosilicate STF among the top three phases by synthesis energy? target: aluminosilicate STF; OSDAs with STF ranked in the top three phases = 13	`stf-candidates` in acs-zeolite-osda-screen	`partial` not-applicable rule applies to negative and inconclusive findings only	informs HYP	record
RES	Which screened or designed OSDAs place aluminosilicate IFR among the top three phases by synthesis energy? target: aluminosilicate IFR; OSDAs with IFR ranked in the top three phases = 5 (n = 18)	`ifr-candidates` in acs-zeolite-osda-screen	`partial` not-applicable rule applies to negative and inconclusive findings only	informs HYP	record
RES	Does de novo design or virtual combinatorial chemistry produce an OSDA with STF among its top three phases by synthesis energy? target: aluminosilicate STF; designed OSDAs near the Pareto front with STF in the top three phases = 0 (n = 18)	`de-novo-stf` in acs-zeolite-osda-screen	`inconclusive-no-positive-control` uninformative no positive control; no negative control; no sensitivity or power statement	consistent-with HYP	record
RES	How well does linear discriminant analysis on volume and Ic separate STF-directing from non-STF OSDAs? target: linear discriminant analysis on volume and Ic (Model 1); sensitivity for STF-directing OSDAs, training set = 92 % (n = 453)	`classifier-model-1` in acs-zeolite-osda-screen	`partial` not-applicable rule applies to negative and inconclusive findings only	informs HYP	record
RES	How well does multilayer perceptron 8-3-2 separate STF-directing from non-STF OSDAs? target: multilayer perceptron 8-3-2 (Model 2); sensitivity for STF-directing OSDAs, training set = 21 % (n = 368)	`classifier-model-2` in acs-zeolite-osda-screen	`partial` not-applicable rule applies to negative and inconclusive findings only	informs HYP	record
RES	How well does multilayer perceptron 8-5-2 trained on chemically similar inactives separate STF-directing from non-STF OSDAs? target: multilayer perceptron 8-5-2 trained on chemically similar inactives (Model 3); sensitivity for STF-directing OSDAs, training set = 42 % (n = 63)	`classifier-model-3` in acs-zeolite-osda-screen	`partial` not-applicable rule applies to negative and inconclusive findings only	informs HYP	record
RES	Did the synthesis-energy prediction for 6-ethyl-1-methyl-5-azaspiro[4.5]decan-5-ium (QHGWEBIGEQBZPY), CHA > AEI > STF, match the phase obtained? target: 6-ethyl-1-methyl-5-azaspiro[4.5]decan-5-ium (QHGWEBIGEQBZPY); predicted phases obtained = 0 (n = 16)	`prediction-qhgwebigeqbzpy` in acs-zeolite-osda-screen	`refuted` not-applicable an affirmative refutation is judged on the refuting analysis, not on the controls of the run it refutes	opposes HYP	record
RES	Did the synthesis-energy prediction for N-benzyl-N,N,2-trimethylpropan-2-aminium (QG001780m), CHA > AEI > IFR, match the phase obtained? target: N-benzyl-N,N,2-trimethylpropan-2-aminium (QG001780m); predicted phases obtained = 0 (n = 12)	`prediction-qg001780m` in acs-zeolite-osda-screen	`refuted` not-applicable an affirmative refutation is judged on the refuting analysis, not on the controls of the run it refutes	opposes HYP	record
RES	Did the synthesis-energy prediction for N-benzyl-N,N-dimethylpropan-2-aminium (QG001780m2), CHA > AEI > IFR, match the phase obtained? target: N-benzyl-N,N-dimethylpropan-2-aminium (QG001780m2); predicted phases obtained = 0 (n = 14)	`prediction-qg001780m2` in acs-zeolite-osda-screen	`refuted` not-applicable an affirmative refutation is judged on the refuting analysis, not on the controls of the run it refutes	opposes HYP	record
RES	Does 6-ethyl-1-methyl-5-azaspiro[4.5]decan-5-ium hydroxide crystallise aluminosilicate STF from an aluminosilicate gel in hydroxide media? target: aluminosilicate STF; syntheses yielding aluminosilicate STF = 0 (n = 16)	`stf-not-formed` in acs-zeolite-stf-synthesis	`inconclusive-no-positive-control` uninformative no positive control; no negative control; no sensitivity or power statement	consistent-with HYP	record
RES	Did 6-ethyl-1-methyl-5-azaspiro[4.5]decan-5-ium (QHGWEBIGEQBZPY) survive the hydrothermal conditions intact? target: 6-ethyl-1-methyl-5-azaspiro[4.5]decan-5-ium (QHGWEBIGEQBZPY); OSDA degradation in the mother liquor = original resonances lost after 30 and 50 days	`osda-degraded` in acs-zeolite-stf-synthesis	`positive` not-applicable rule applies to negative and inconclusive findings only	supports HYP	record

Issues (7 open questions and untried branches)

ISS Can aluminosilicate STF or IFR be crystallised in hydroxide media at all, given that CHA and AEI are predicted to be more stable for every OSDA screened? (open-question)
ISS Would the predicted phases (CHA, AEI) have formed if the OSDAs had survived the hydrothermal conditions? (open-question)
ISS Include solvent effects, especially how water and counter-cations influence framework stability and OSDA-framework interaction, in the phase prediction. (proposed-by-authors)
ISS Examine OSDA stability under hydrothermal conditions, since degradation during synthesis can prevent structure direction. (proposed-by-authors)
ISS Link computational insight with experimental feedback to guide zeolite crystallisation. (proposed-by-authors)
ISS Run one of the 36 OSDAs known to direct pure-silica STF through the same hydroxide aluminosilicate protocol, as a positive control for the protocol. (inferred-by-ingest)
ISS Synthesise and test the ten shortlisted candidates in SI Tables S14 to S17 that were not taken to the bench. (inferred-by-ingest)