不对称双位点Bi-In氧桥用于高效光热催化二氧化碳甲烷化

doi:10.1016/S1872-2067(25)64922-9

催化学报 ›› 2026, Vol. 83: 351-362.DOI: 10.1016/S1872-2067(25)64922-9

不对称双位点Bi-In氧桥用于高效光热催化二氧化碳甲烷化

郑芒^a, 李琪^a, 刘倩茜^b, 谷慧泉^b, 刘明阳^a, 刘琦^a^,^*(), 蒋保江^a^,^b^,^*()

^a哈尔滨工程大学材料科学与化学工程学院, 超轻材料与表面技术教育部重点实验室, 黑龙江哈尔滨 150001
^b黑龙江大学化学与材料科学学院, 功能无机材料化学教育部重点实验室, 黑龙江哈尔滨 150080

收稿日期:2025-08-06 接受日期:2025-10-11 出版日期:2026-04-18 发布日期:2026-03-04
通讯作者: * 电子信箱: qiliu@hrbeu.edu.cn (刘琦), jbj@hlju.edu.cn (蒋保江).
基金资助:
国家自然科学基金(U24A20550);国家自然科学基金(52273264);黑龙江省自然科学基金重点项目(ZD2024B001)

Asymmetric oxygen-bridged Bi-In dual sites for efficient photothermal CO₂ methanation

Mang Zheng^a, Qi Li^a, Qianxi Liu^b, Huiquan Gu^b, Mingyang Liu^a, Qi Liu^a^,^*(), Baojiang Jiang^a^,^b^,^*()

^aKey Laboratory of Superlight Materials and Surface Technology, Ministry of Education, College of Materials Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, Heilongjiang, China
^bKey Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People's Republic of China, School of Chemistry and Materials Science, Heilongjiang University, Harbin 150080, Heilongjiang, China

Received:2025-08-06 Accepted:2025-10-11 Online:2026-04-18 Published:2026-03-04
Contact: * E-mail: qiliu@hrbeu.edu.cn (Q. Liu), jbj@hlju.edu.cn (B. Jiang).
Supported by:
National Natural Science Foundation of China(U24A20550);National Natural Science Foundation of China(52273264);Key Project of the Heilongjiang Provincial Natural Science Foundation(ZD2024B001)

摘要/Abstract

摘要：

利用太阳能将二氧化碳(CO₂)光催化转化为高附加值化学品, 被认为是解决环境问题和能源危机的有效策略之一, 为可持续发展提供了巨大潜力. 其中, CO₂的甲烷化因其在能源存储和工业原料方面的双重用途而备受关注. 然而, 以水(H₂O)为质子源, 将CO₂光催化还原为甲烷(CH₄)的效率较低, 这主要是由于该过程涉及C=O键活化和H₂O分解过程的固有热力学限制. 光热协同催化策略通过降低反应活化能垒在一定程度上提升了CO₂的转化效率, 但同时实现高CH₄产率和选择性仍然面临挑战. 这主要源于CO₂还原和析氢反应(HER)之间的竞争, 以及反应中间体在催化剂表面的弱吸附. 因此, 在光热CO₂甲烷化中, 开发能够有效抑制HER并调控反应中间体的催化剂是实现高CH₄产率和选择性的关键.
本研究通过将Bi原子精准锚定于In₂O₃晶格, 构建了结构明确的氧桥联不对称双金属位点(In-O-Bi). 该结构充分利用p区元素固有的弱质子吸附特性, 有效抑制了竞争性HER, 为实现高效的光热催化CO₂甲烷化过程奠定了材料基础. In-O-Bi位点的成功构建得到了多种结构表征的协同验证: X射线衍射结果证实了Bi³⁺对In₂O₃晶格的掺入; 高分辨透射电镜从实空间证明了Bi的原子级分散; X射线光电子能谱分析则通过In 3d谱图中特征峰的结合能位移揭示了Bi与In之间的电子相互作用; 而扩展X-射线吸收精细结构分析最终从原子局域结构上确认了In-O-Bi单元的存在. 在CO₂和H₂O的混合气氛中, Bi/In₂O₃催化剂表现出卓越性能, 甲烷产率达到214.1 μmol·g^-1, 选择性高达96.7%. 其高性能源于多种机制的协同, 一方面, Bi与In之间的p轨道杂化有效抑制了HER并削弱了*H中间体的表面吸附; 另一方面, 独特的In-O-Bi桥联构型诱导产生显著的电子离域效应, 促使高活性催化中心的形成. 在该结构中, Bi位点表现出与CO₂分子的强相互作用及电子供给能力, 而In位点则具有较低的水分子解离能垒. 此外, In-O-Bi结构的形成增强了催化剂对CO₂和H₂O的吸附能力, 其电子离域效应也促进了对关键CHO物种的吸附稳定与电子转移过程, 从而显著降低整个反应路径的能垒, 最终实现高效、高选择性的CO₂至CH₄转化.
综上, 本文通过构建In-O-Bi桥联结构, 利用p区金属间的协同作用有效抑制了竞争性HER反应, 并通过p轨道杂化诱导的电子离域效应, 成功实现了CO₂向高附加值甲烷的高效转化. 该发现为设计高性能光热催化剂提供了重要见解, 凸显了氧桥联不对称双金属单元在推动CO₂甲烷化及可持续能源技术发展方面的巨大潜力.

关键词: 光热催化, 二氧化碳甲烷化, 轨道杂化, 电子离域化, In-O-Bi桥位点

Abstract:

Photothermal coupling catalytic CO₂/H₂O to CH₄ is recognized as an effective strategy for addressing environmental concerns and energy crisis. However, hydrogen evolution reaction (HER) competition and weak intermediate adsorption limiting CH₄ selectivity and yield during the reaction process. Herein, we incorporate Bi into the In₂O₃ lattice to create an oxygen-bridged asymmetric bimetallic In-O-Bi (In-O-Bi bridge) sites. The optimized Bi/In₂O₃ catalyst achieves CH₄ yield of 214.1 μmol·g^-1 with 96.7% selectivity. The exceptional catalytic activity of Bi/In₂O₃stems from two key synergistic effects: (1) the cooperative interaction between Bi and In as p-block metals effectively suppress the competing HER, and (2) the unique In-O-Bi bridge configuration induces significant electron delocalization through p-orbital hybridization. This electronic modulation creates highly active catalytic centers, with In sites preferentially facilitating H₂O dissociation while Bi sites selectively promote CO₂ reduction. Moreover, the electron delocalization effect in the In-O-Bi bridge sites enhances the adsorption and electron transfer capabilities of the Bi/In₂O₃ surface for key CHO species, and reduces the energy barrier, thereby enabling efficient CH₄ production. These findings provide crucial insights into the design of photothermal catalysts, highlighting the transformative potential of oxygen-bridged asymmetric bimetallic units in efficient CO₂ methanation and sustainable energy technologies.

Key words: Photothermal catalysis, CO₂ methanation, Orbital hybridization, Electron delocalization, In-O-Bi bridge sites

郑芒, 李琪, 刘倩茜, 谷慧泉, 刘明阳, 刘琦, 蒋保江. 不对称双位点Bi-In氧桥用于高效光热催化二氧化碳甲烷化[J]. 催化学报, 2026, 83: 351-362.

Mang Zheng, Qi Li, Qianxi Liu, Huiquan Gu, Mingyang Liu, Qi Liu, Baojiang Jiang. Asymmetric oxygen-bridged Bi-In dual sites for efficient photothermal CO₂ methanation[J]. Chinese Journal of Catalysis, 2026, 83: 351-362.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(25)64922-9

https://www.cjcatal.com/CN/Y2026/V83/I4/351

图/表 5

Fig. 1. (a) Schematic representation of the synthesis of Bi/In2O3. (b) Rietveld refinement of the XRD pattern structure of Bi/In2O3. (c) SEM. (d) TEM. (e) A high-resolution TEM. (f) HADDF-STEM and corresponding elemental mapping images of Bi/In2O3.

Fig. 2. In 3d (a) and Bi 4f (b) XPS spectra. (c) Normalized Bi L3-edge XANES spectra with Bi2O3 and Bi foil references. (d) Average Bi valence state in Bi/In2O3. (e) k2-weighted Bi L3-edge Fourier transform EXAFS spectra with references. (f) Bi L-edge EXAFS data (line) and best fits (circles) for Bi/In2O3 in k2-weighted r-space. (g-i) wavelet-transform EXAFS images of Bi/In2O3, Bi2O3, and Bi foil.

Fig. 3. (a) Temporal evolution of CO2 reduction products over In2O3 and Bi/In2O3. (b) Activation energies of catalysts under photothermal conditions. (c) Product distribution for Bi/In2O3 series. (d) Electron participation and O2 evolution comparison during methanation. (e) The cycling tests of Bi/In2O3 sample. The aforementioned experiments were conducted at 300 °C with 1.77 W·cm-2. (f) Product distribution under various conditions (10 h). (g) Under constant reaction temperature (573 K), the trend of product variation with light intensity. (h) Activation energies of Bi/In2O3 under photothermal catalysis and Thermal catalysis conditions. (i) Under constant light intensity (1.77 W·cm-2), the trend of product variation with temperature. Data are presented as the mean ± standard deviation from three independent experiments, significance was defined as p≤0.05.

Fig. 4. (a) Photothermal CO2 methanation reaction under various conditions. (b) GC-MS spectrum of the products in photothermal 13CO2 and D2O methanation reaction. (c,d) CO2-TPD and H2O-TPD spectra of In2O3 and Bi/In2O3. In-situ DRIFTS of spectra of In2O3 (e) and Bi/In2O3 (f) during H2O and CO2 adsorption. In-situ DRIFTS spectra of In2O3 (g) and Bi/In2O3 (h) under visible light and 300 °C after adsorption saturation. (The “ads” represents surface adsorbed states.)

Fig. 5. (a,b) The projected density of states (PDOS) of Bi/In2O3 and In2O3 model in *CO2 states. (c) Free energy profile for the HER process on Bi/In2O3 and In2O3 model. (d) PDOS of Bi/In2O3 and In2O3 model after *H adsorption. (e,f) Electronic location function results. (g) Energy barrier for H2O dissociation on the In and Bi sites of Bi/In2O3. (h,i) Charge density difference of CHO species on In2O3 and Bi/In2O3 model. Yellow and blue represent electron accumulation and depletion, respectively. (j) Illustration of the mechanism of photocatalytic CO2 reduction and H2O oxidation on Bi/In2O3.

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不对称双位点Bi-In氧桥用于高效光热催化二氧化碳甲烷化

Asymmetric oxygen-bridged Bi-In dual sites for efficient photothermal CO₂ methanation

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不对称双位点Bi-In氧桥用于高效光热催化二氧化碳甲烷化

Asymmetric oxygen-bridged Bi-In dual sites for efficient photothermal CO2 methanation

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Asymmetric oxygen-bridged Bi-In dual sites for efficient photothermal CO₂ methanation