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Many organic molecules with various functional groups have been used to passivate the perovskite surface for improving the efficiency and stability of perovskite solar cell (PSCs).However,the intrinsic attributes of the passivation effect based on different chemical bonds are rarely studied.Here,we comparatively investigate the passivation effect among 12 types of functional groups on para-tertbutylbenzene for PSCs and find that the open circuit voltage (Voc) tends to increase with the chemical bonding strength between perovskite and these passivation additive molecules.Particularly,the paratert-butylbenzoic acid (tB-COOH),with the extra intermolecular hydrogen bonding can stabilize the surface passivation of perovskite films exceptionally well through formation of a crystalline interlayer with water-insoluble property and high melting point.As a result,the tB-COOH device achieves a champion power conversion efficiency (PCE) of 21.46％.More importantly,such devices,which were stored in ambient air with a relative humidity of ≈45％,can retain 88％ of their initial performance after a testing period of more than 1 year (10,080 h).This work provides a case study to understand chemical bonding effects on passivation of perovskite.