The
self-reduction mechanism in pyrophosphate phosphors is currently
explained through nonequivalent substitution for charge compensation.
Nevertheless, the impact of oxygen vacancies on the self-reduction
enhancement requires further investigation. Herein, heterovalent Ba1–x
Zn1–y
P2O7:xEu2+/3+, yMg phosphors with rigid structures were prepared
through conventional solid-phase technology in air. The cation substitution
strategy leads to different chemistry electronegativity and adjustable
crystal field environments and creates vacancy defects. Crystal structure
and component analysis indicate the gradual phase segregation change
from BaZnP2O7 to BaMgP2O7 with increasing Mg2+ content. The CIE coordinates that
are tuned from (0.514, 0.334) to (0.326, 0.152) and realize color-tunable
emission from red-orange to blue-violet can be used as multicolor
functional materials. Besides, the phosphor demonstrates its maximum S
a of 0.4725% K–1 (498 K) and S
r of 1.376% K–1 (423 K). These
results demonstrate that the phosphors have the potential for contactless
optical temperature measurement and anticounterfeiting. This work
not only investigates the self-reduction of the Eu3+ →
Eu2+ phenomenon but also provides a supplementary explanation
and data support to complete the effect of the oxygen vacancy on self-reduction.