Inverted perovskite
solar cells (PSCs) have attracted intense attention
because of their insignificant hysteresis and low-temperature fabrication
process. However, the efficiencies of inverted PSCs are still inferior
to those of commercialized silicon solar cells. Also, the poor stability
of PSCs is one of the major impedances to commercialization. Herein,
we rationally designed and synthesized a new series of electron donor
(
R
,
R
-diphenylamino) and acceptor
(pyridimium-(CH
2
)
n
-sulfonates)
zwitterions as a boundary modulator and systematically investigated
their associated interface properties. Comprehensive physical and
optoelectronic studies verify that these zwitterions provide a four-in-one
functionality: balancing charge carrier transport, suppressing less-coordinated
Pb
2+
defects, enhancing moisture resistance, and reducing
ion migration. Although each functionality may have been reported
by specific passivating molecules, a strategy that simultaneously
regulates the charge-transfer balance and three other functionalities
has not yet been developed. The results are to make an omnidirectional
improvement of PSCs. Among all zwitterions, 4-(4-(4-(di-(4-methoxylphenyl)amino)phenyl)propane-1-ium-1-yl)butane-1-sulfonate
(OMeZC3) optimizes the balance hole/electron mobility ratio of perovskite
to 0.91, and the corresponding PSCs demonstrate a high power conversion
efficiency (PCE) of up to 23.15% free from hysteresis, standing out
as one of the champion PSCs with an inverted structure. Importantly,
the OMeZC3-modified PSC exhibits excellent long-term stability, maintaining
almost its initial PCE after being stored at 80% relative humidity
for 35 days.