SUPPORTING INFORMATION

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1 SUPPORTING INFORMATION Pickering Emulsion Formation of Paraffin Wax in an Ethanol-Water Mixture Stabilized by Primary Polymer Particles and Wax Microsheres Thereof Zuoxu Xiao, Hongyan Cao, Xubao Jiang*, Xiang Zheng Kong* College of Chemistry and Chemical Engineering, University of Jinan, Jinan , China Corresonding authors s: S1

2 1. Contact Angles and Adsortion Energy: Contact angles of H 2 O-EtOH mixture on solid ax and on PPs film ere measured using goniometer (OCA-40, Datahysics, Germany). Wax film as reared as folloing: 5 g of solid araffin ax as ut in a culture dish and heated at 75 C till the ax melted, and a liquid layer of ax formed. A thin film of solid ax as obtained soon after the heating halted. The thin ax film as cut to squares (about 1 cm 2 ). For the olymer film of P(DC-TMPTA), ethylbenzene (1 ml) as dro-ise added into 0.2 g of olymer microsheres, after ell mixed, the mixture as located into a ater bath at 50 C the olymer microsheres ere alloed to soll for 0 min to obtain a viscous mixture, hich as taken using a iette and laced on a glass slide. A olymer film as formed after the solvent evaorated. Contact angles of ater, ethanol, their mixture and liquid ax on the surface of the P(DC-TMPTA) film and on solid ax ere determined. The interface tension beteen liquid ax and EtOH-H 2 O as determined ith an interfacial rheometer (Tracker-H, Teclis, France) folloing a reorted rocedure (Anton, N.; Vandamme, T. F.; Bouriat, P. Dilatational rheology of a gel oint netork formed by nonionic soluble surfactants at the oil ater interface. Soft Matter 201, 9, ). 2. Evolution of Granular Proerty of P(DC-TMPTA) Primary Particles. Table S1. Evolutions of size and size distribution of PPs in reciitation olymerization of TMPTA-DC Polymerization time (h) D n (μm) PDI (D /D n ) Otical Microscoe Photos of Wax Sheres Preared under Different Conditions. S2

60 (Conditions: 70 ºC, 4.0 g of ax and 0.4 g of PPs in 100 g of EtOH-H 2 O mixture ith 10 t% of H 2 O.) Figure S2.

3 Figure S1. OM ictures of the ax microsheres reared in EtOH-H 2 O mixture ith different shaking rate (osc/min): A, 240; B, 280; C, 20; D, 60 (Conditions: 70 ºC, 4.0 g of ax and 0.4 g of PPs in 100 g of EtOH-H 2 O mixture ith 10 t% of H 2 O.) Figure S2. OM ictures of the ax microsheres reared in EtOH-H 2 O mixture ith different amount of olymer articles: A, 0.2 g; B, 0.4 g; C, 0.8 g; D, 1.0 g. (Conditions: 70 ºC; shaking at 20 osc/min; 4.0 g of ax in 100 g of EtOH-H 2 O mixture ith 10 t% of H 2 O.) S

4 4. Number of Small Polymer Particles Adhered on Wax Microsheres. In the system, the total mass of the large ax microsheres (ith average radius of R ) is denoted as m t, its number denoted as n, the mass of a single ax microshere denoted as m s ; the total mass of the olymer articles (ith the average radius of r ), found together ith the ax sheres, is denoted as m t, its number denoted as n, the mass of a single olymer article denoted as m s. The folloing equations are established: n m m m (1) t t s 4 R n m m t t (2) m 4 r s Where, ρ and ρ are the density of the ax and the P(DC-TMPTA), i.e. oly(dodecene-and trihydroxymethyl roane triacrylate). From these equations, it is easy to calculate the exerimental number (N ex ) of the olymer articles adsorbed or engulfed by each ax microshere, as exressed by Eq. (): N ex n m R () n t mtr Knoing that the surface area (S s ) of a single ax microshere is exressed by Eq. (4): S s =4πR 2 (4) Simly dividing the surface area (S s, Eq. 4) of a single ax microshere by the number of the olymer article (N ex, Eq. ) er ax shere, the exerimental average surface area occuied by each olymer article on the surface of the ax sheres (S ex ) is exressed by Eq. 5, regardless of the location of the olymer articles, i.e. hether they ere adsorbed ith mono- or multi-layer on the surface of, or artially engulfed in the ax sheres. S4

5 S ex S 4 m s tr (5) N m R ex t It is obvious that the number of small olymer articles found ith a large ax microshere, i.e., N ex given by Eq. (), is obtained simly by dividing the olymer articles (n, Eq. 2), exerimentally found ith a large ax microshere, by the number of ax sheres (n, Eq. 1), and the average surface area (S ex, Eq. 5) occuied by one single olymer article on the ax shere surface is obtained simly by dividing the surface area of a single ax microshere (S s, Eq. 4) by the number of the olymer articles (N ex, Eq. ) adsorbed on or engulfed by each ax microshere. These values, i.e., n in Eq. 2 and S ex in Eq. 5, can be regarded as exerimental values because they are estimated simly based on the amounts of the olymer articles and the ax microsheres and their sizes (R and r ). On the other hand, a theoretical area (denoted as S min, Eq. 6) occuied by a olymer article can also be calculated by assuming that the small articles are closely acked on the ax surface as illustrated in Figure S. Comaring this theoretical S min ith the exerimental surface area S ex, one can see ho the ax shere surface is covered by the small articles. Figure S. Schematic vies of tightly acked small olymer articles on the surface of a large ax microshere. (A: Vie of a dissected section of a ax shere ith closely acked olymer articles on its surface; B: Exterior vie of a ax shere ith closely acked olymer articles on its surface; C: Enlarged vie of closely acked olymer articles on the surface of a large ax shere.) S5

6 S min S 2 R s r Nmax R r (6) Where N max is the maximal number of the small olymer articles that a large ax microshere can take under tightly acking as shon in Figures S. N max is obtained from Eq. (7). N 4 ( R r ) / 2 max 2 R r r 2 r (7) Detail for the rocess of the deduction for the equations (6) and (7) has been described in full in a revious ublication (Cao, H.; Zhang, L.; Wu, L.; Kong, X. Z. Characterization of Heterocoagulation ith Oositely Charged Polymer Colloid Particles through Online Tracking of Light Transmittance. ACS Al. Mater. Interfaces 2016, 8, ). Here given is a brief descrition. 5. Estimation of PPs Number on Wax Microsheres. Table S2. Exerimental (N ex ) and theoretical (N max ) numbers of PPs adsorbed and the corresonding exerimental (S ex ) and theoretical (S min ) areas of a single olymer article occuied on a single ax shere reared ith different amount of PPs articles Polymer articles (g) PPs/Wax (t%) N ex (PPs on ax shere) N max (PPs on ax shere) S ex (μm 2, PP area ext.) S min (μm 2, PP area theo.) S6

Nondestructive Monitoring of Setting and Hardening of Portland Cement Mortar with Sonic Methods

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