Influence of Structural Disorders on the Tribological Behavior of Phosphate-Intercalated Layered Double Hydroxide Additives in Polyalphaolefin

In this work, several phosphate-intercalated Mg-Al layered double hydroxides (LDHs) were synthesized and evaluated as solid lubricant additives in polyalphaolefin (PAO-4) by means of tribotesting on coupled GCr15/cast iron contacts. The effects of test parameters such as normal loads, additive concentrations, and substrate surface roughness were investigated, while the LDH crystal structure received considerable attention. Several types of structural disorder after anion exchange were identified based on X-ray diffraction (XRD) analysis. The unstable structures promote feasible shearing during sliding to improve friction and wear. In addition, antiwear properties correlate well with the anion charge number or the quantity of anion in the interlayer region. Overall, the tribological performance increased in the order HPO42--LDH < PO43--LDH < P2O74--LDH < (PO3)(6)(6-)-LDH. (PO3)(6)(6-)-LDH demonstrated the best antiwear performance with a reduction of 69% of the ball volume loss compared to PAO-4 oil due to the synergy of the disordered stacking LDH sheets and flexible ring structure of the (PO3)(6)(6-) anion. Furthermore, on polished surfaces, the coefficient of friction (COF) of the (PO3)(6)(6-)-LDH sample dropped significantly by 26%, while the wear loss reduction of more than 80% was also substantial compared to the base oil sample. A performance comparison between the best-performing LDH additive was also conducted against popular nanomaterials, such as hexagonal boron nitride (BN), graphene nanoplatelets (GNPs), and titanium oxide (TiO2). The performance of (PO3)(6)(6-)-LDH was close to that of GNPs.