Digitizing protocols into single reactors for the one-pot synthesis of nanomaterials

•One-pot one-time, dropwise, and sequential addition syntheses of nanomaterials•Encodes synthetic procedures into reactor using chemical description language χDL•Synthesis CdSe QDs, [email protected] core-shell NPs, Pt-Fe3O4 Janus NPs•Simple, reproducible, accessible for automated synthesis nanomaterials Nanomaterials exhibit unique properties that are tunable based on morphology composition. However, commonly used may lack complete or accurate knowledge, leading to a reproducibility crisis. To address this, we have developed new approach encodes single reactor. Our proof-of-concept automation, which does not rely electronic components, is demonstrated in the one-pot quantum dots, nanoparticles, nanoparticles. As materials science continues advance, anticipate capabilities can be further expanded by cost-efficient environmentally friendly functional materials. This offers simple, reliable, reproducible method nanoparticle synthesis, easily adapted researchers different fields. depending their widely methods fail due incomplete assumed knowledge protocol. A digital could unambiguously capture process, including required hardware, reagent inputs, process description, thereby increasing accessibility improving reproducibility. reactors imprinting parameters reactor’s morphology, described language, χDL. consolidated three automate complex processes such as eight time-resolved respectively. translating physical instances enables automation nanomaterial manner, making from various fields demand. Nanomaterials, synthesized colloidal dispersion, been utilized variety electro-, opto-magneto-, mechano-, thermal, chemo-devices,1Kovalenko M.V. Manna L. Cabot A. Hens Z. Talapin D.V. Kagan C.R. Klimov V.I. Rogach A.L. Reiss P. 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Digital metal–organic frameworks.Angew. 57: 16716-16720https://doi.org/10.1002/anie.201810095Crossref (14) In latter example, precursors were compartmentalized mixed at high temperatures upon manually flipping oven, reactivity. hypothesis digitalized geometry self-contained reactors, produced, Herein, protocols descriptions sealed reactors. manufactured combining polymeric thermal separate precursor solutions compartments prevent early unwanted reactions. combination polymers endure desired polypropylene [PP] polyether-ether-ketone [PEEK]) composite continually optimized synthesis. achieved high-temperature (i.e., PEEK) body low-temperature seals made polycaprolactone [PCL]) compartments. pre-loaded reactor, then placed pre-heated oven where break programmed temperature initiate reaction. compartmentalization incorporated designs utility was nanocrystals, general traditional enclosed design unlock chemistry across research provide inexperienced safe, low-cost, access nanomaterials. 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During reaction, temperatures; thus, contain chambers (two reagents one compartment), separated temperature-sensitive seal PCL, shown Figure 1. custom-made than PP (m.p. = 63°C, revealed differential scanning calorimetry [DSC]; see S1), allowing polymer soften eventually temperatures. Heating cartridge (130°C) allowed drop compartment Initially, disk-shaped 2A) during solutions. Varying width when compartment. transferred chamber after 10 (ca. 70°C), 15 90°C), 25 min 0.5, 1, 2 mm seals, Considering starts 130°C, thickness provides appropriate timing mixed. use septa under atmosphere (see supplemental preparation procedure). loaded aliquots taken 1 h intervals syringes long needles. resulted irreproducible photoluminescence (PL) emissions formed 2G (yellow square trace) shows differences large ±17 nm between batches second (after respectively). suggest uneven breaking seal, continuous mixture instead one-time generating nucleation stages. cone-shaped designed, focusing pressure point middle section 2B). carved-in cone total height 4 bottom maintain temperature. more PL sample (±6 compared obtained design; 2G). nanocrystal still showed significant (±14 nm), most likely distribution batches. analyze computational fluid dynamics (CFD) simulations performed S2). cross-section region 130°C Figures 2D 2E. disk- highest membrane located toward outside edge (104°C), ΔT ca. 19°C. difference suggests even if there design, determined slow heat PCL. Knowing focused external locate outer (slide-shaped 2C 2F). slide-shaped mm, slope 24°, mm. cartridge, facing wall being batches, minimizing error bars ± 3 Consistent results triplicates 9 replicates) glassware 2H) indicating standard reducing human input, reproducible. time-evolution profile (NC) monitored UV-visible (UV-vis) fluorescence spectroscopy each aliquot (0.5 mL) sampled mixtures. absorption emission spectra injection grow (Figures 3A 3B ). When NCs stage formation (<1 injection), broadband dominates surface-to-volume ratio. grow, band becomes prominent emission, narrower peaks. absorbance typically show peak centered around 412 nm, magic-size clusters.30Yu M.Z. Wang Piolet M.L. Frotey Zaman M.B. Wu X. Leek D.M. Tao Wilkinson Li Thermodynamic equilibrium-driven single-sized nanocrystals: media tuning magic-sized versus regular dots.J. 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PPcomm decent adhesion property good sealing preventing leaking chambers. PEEK/PPcomm (body/seal) perform higher (180°C). CFD simulations, 180°C, 140°C S3). same techniques PP/PCL systems (PP/PCL vs. PEEK/PPcomm) timescale. While 3.2 PEEK/PP little size. reason, monitor growing NCs, 5 3C). At temperatures, thermally driven, thus no corresponding clusters. 3C how redshifted continuously reaction; growth, FWMH 43 nm. elevated (180°C), reach 2.6 130°C. core usually covered shell high-energy gap ZnS, ZnSe, CdS) efficiency. Introducing shells prevents electron-hole recombination caused dangling bonds.33Vasudevan Gaddam R.R. Trinchi Cole I. Core–shell Alloys Compd. 636: 395-404https://doi.org/10.1016/j.jallcom.2015.02.102Crossref (212) add NC, reactions two-step form containing cores. avoid homogeneous nucleation, added dropwise. Among coat cores, ZnSe highly desirable it interfacial misfits turn traps electrons holes. imprint base need (as depicted First, two 190°C, critical step, dropwise must adding precursor. blueprint principle Soxhlet extractor. connected solution reservoir, via U-tube siphon 4A S5). adaptor end tubing addition. carried out resistance, seal. features 4A. test perylene set 190°C. Aliquots every min, collected started, showing concentration increases over 4B). sampling completed once values plateaued, matching diluted stock (5 mM). elapsed volume added, 0.2 mL/min. determining QD hour growth. 4C, small bathochromic shift UV spectra. deviation 1.5 (Table S2), showcasing system. Seed-mediated successful shapes noble reliability versatility.34Niu Xu crystal control.Nanoscale. 2013; 5: 3172-3181https://doi.org/10.1039/C3NR00219ECrossref involves reduction synthesize morphologies Janus, dumbbell, shell, etc.).35Murphy Sau Gole A.M. 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