Tailored DynamicSeesaw Configuration of Heterojunctionsto Enhance Piezo-Photocatalytic Overall Nitrogen Fixation

Relay overall nitrogen fixation presents an intriguing approach to the simultaneous production of nitric acid and ammonia. However, it remains a significant challenge due to manipulating dual active sites on both temporal and spatial mesoscopic scales. In this study, we propose a bionic seesaw Bi<sub>4</sub>O<sub>5</sub>Cl<sub>2</sub>−Bi<sub>4</sub>O<sub>5</sub>Br<sub>2</sub> heterojunction, which establishes a one-way reaction channel through the entanglement effect, challenging the inherent idea of synchronous reaction in a heterojunction. Notably, the adaptive interface functions as a fulcrum by incorporating both tensile Bi−Cl bonds and compressive Bi−Br bonds while also inducing the localized surface lattice distortion of Bi−O to sequentially activate the active sites. Therefore, unsaturated sites and dynamic properties trigger the seesaw structure to enhance both charge exchange and molecular polarization of N<sub>2</sub> during reduction, thereby creating a hydroxy-rich environment for the ammonia oxidation process. Our work offers a novel active site control perspective and clarifies nitrogen fixation processes.

Publication Details

Journal
Figshare
Published
2025-02-03
DOI
https://doi.org/10.1021/acs.nanolett.4c06083.s001
Primary Topic
Ammonia Synthesis and Nitrogen Reduction
Type
article
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article

Tailored DynamicSeesaw Configuration of Heterojunctionsto Enhance Piezo-Photocatalytic Overall Nitrogen Fixation

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Ammonia Synthesis and Nitrogen Reduction
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Tailored DynamicSeesaw Configuration of Heterojunctionsto Enhance Piezo-Photocatalytic Overall Nitrogen Fixation

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Abstract

Relay overall nitrogen fixation presents an intriguing approach to the simultaneous production of nitric acid and ammonia. However, it remains a significant challenge due to manipulating dual active sites on both temporal and spatial mesoscopic scales. In this study, we propose a bionic seesaw Bi<sub>4</sub>O<sub>5</sub>Cl<sub>2</sub>−Bi<sub>4</sub>O<sub>5</sub>Br<sub>2</sub> heterojunction, which establishes a one-way reaction channel through the entanglement effect, challenging the inherent idea of synchronous reaction in a heterojunction. Notably, the adaptive interface functions as a fulcrum by incorporating both tensile Bi−Cl bonds and compressive Bi−Br bonds while also inducing the localized surface lattice distortion of Bi−O to sequentially activate the active sites. Therefore, unsaturated sites and dynamic properties trigger the seesaw structure to enhance both charge exchange and molecular polarization of N<sub>2</sub> during reduction, thereby creating a hydroxy-rich environment for the ammonia oxidation process. Our work offers a novel active site control perspective and clarifies nitrogen fixation processes.

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Ammonia Synthesis and Nitrogen Reduction
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Tailored DynamicSeesaw Configuration of Heterojunctionsto Enhance Piezo-Photocatalytic Overall Nitrogen Fixation · Figshare (2025) | TGRS Research Map | TGRS