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Direct spectroscopic evidence for a hydride bridge in the Ni–R form of [NiFe] hydrogenase has been obtained using iron‐specific nuclear resonance vibrational spectroscopy (NRVS). The Ni–H–Fe wag mode at 675 cm−1 is the first spectroscopic evidence for a bridging hydride in Ni–R as well as the first iron‐hydride‐related NRVS feature observed for a biological system. Although density function theory...
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