In Situ Metal‐Oxygen‐Hydrogen Modified B‐Tio2@Co2P‐X S‐Scheme Heterojunction Effectively Enhanced Charge Separation for Photo‐assisted Uranium Reduction
In Situ Metal‐Oxygen‐Hydrogen Modified B‐Tio2@Co2P‐X S‐Scheme Heterojunction Effectively Enhanced Charge Separation for Photo‐assisted Uranium Reduction
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原位金属-氧-氢改性B-TiO 2 @ Co2 P-XS-Scheme异质结有效增强光助铀还原的电荷分离
DOI：
10.1002/advs.202305439
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发表时间：
2023-12
期刊：
影响因子：
15.1
通讯作者：
Fucheng Zhang;Huanhuan Dong;Yi Li;Dengjiang Fu;Lu Yang;Yupeng Shang;Qiuyang Li;Yuwen Shao-Yuwen-Sha
中科院分区：
文献类型：
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作者：
Fucheng Zhang;Huanhuan Dong;Yi Li;Dengjiang Fu;Lu Yang;Yupeng Shang;Qiuyang Li;Yuwen Shao-Yuwen-Sha
光辅助铀还原有望克服传统工艺中杂质离子与U（VI）之间的竞争。在这里，开发了具有金属-氧-氢（M-O-H）的B-TiO 2@Co2 P-X S-方案异质结，用于光辅助U（VI）（六价铀）还原。基于密度泛函理论和Hard-Soft-Acid-Base（HSA B）理论，发现在B-TiO 2 @ Co2 P-X中引入金属-氧-氢（M-O-H，硬碱）金属键可以增强亲水性和对铀酰离子（硬酸）的捕获能力。因此，B-TiO2@Co2P-500杂化纳米片在竞争离子的存在下表现出优异的U（VI）还原能力（>98%）。通过自洽能带计算和原位KPFM光谱分析，证实了B‐ TiO 2和Co2 P之间在异质结处形成了内电场，为加速S‐图式载流子定向迁移和促进铀的光催化还原提供了强大的驱动力和原子运输高速公路。本工作为探索具有高效光电子分离功能的光催化剂还原U（VI）提供了一条有价值的途径。
Photo‐assisted uranium reduction from uranium mine wastewater is expected to overcome the competition between impurity ions and U(VI) in the traditional process. Here, B‐TiO2@Co2P‐X S‐scheme heterojunction with metal‐oxygen‐hydrogen (M‐O‐H) is developed insitu modification for photo‐assisted U(VI) (hexavalent uranium) reduction. Relying on the DFT calculation and Hard‐Soft‐Acid‐Base (HSAB) theory, the introduction of metal‐oxygen‐hydrogen (M‐O‐H, hard base) metallic bonds in the B‐TiO2@Co2P‐X is found to enhance the hydrophilicity and the capture capability for uranyl ion (hard acid). Accordingly, B‐TiO2@Co2P‐500 hybrid nanosheets exhibit excellent U(VI) reduction ability (>98%) in the presence of competing ions. By self‐consistent energy band calculations and in‐situ KPFM spectral analysis, the formation of the internal electric field between B‐TiO2 and Co2P at the heterojunction is proven, offering a strong driving force and atomic transportation highway for accelerating the S‐scheme charge carriers directed migration and promoting the photocatalytic reduction of uranium. This work provides a valuable route to explore the functionally modified photocatalyst with high‐efficiency photoelectron separation for U(VI) reduction.