NaBH4 辅助合成 B-(Ni-Co)/MgAl2O4 纳米结构用于甲烷催化干法重整,ACS Applied Nano Materials

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NaBH4 辅助合成 B-(Ni-Co)/MgAl2O4 纳米结构用于甲烷催化干法重整
ACS Applied Nano Materials ( IF 5.3 ) Pub Date : 2022-07-19 , DOI: 10.1021/acsanm.2c02213
Md Shakir _{1,

2} , Manohar Prasad ₂ , Koustuv Ray ₃ , Siddhartha Sengupta ₂ , Apurba Sinhamahapatra ₂ , Shaomin Liu ₁ , Hari Babu Vuthaluru ₁

Affiliation

催化剂表面上的碳沉积不利于甲烷的干重整 (DRM) 反应。发现添加硼 (B) 可有效降低碳沉积。_{在这项研究中，通过 NaBH 4}还原方法合成了具有不同 Ni/Co 比的MgAl ₂ O ₄ (MA) [B-(Ni-Co)/MA] 上的双金属 Ni、Co 催化剂，并在 600 °C 下检测了 DRM。和大气压。NaBH ₄在一步催化剂制备方法中，在将金属盐还原为金属、掺入 B 和增强活性金属物质的分散方面起着至关重要的作用。在 MA 的二维薄片上观察到棒状 Ni-Co 合金和 B-(Ni-Co) 纳米结构。与其他制备的催化剂相比，富镍含 B 双金属 [B-(75Ni-25Co)] 催化剂表现出更好的甲烷和二氧化碳转化率。周转频率（CH ₄)和B催化剂的合成气比分别是相同Ni/Co比下传统浸渍法制备的非B催化剂的1.5倍和1.04倍。催化剂 [B-(75Ni-25Co)] 表现出更高的活性和几乎稳定的转化率，而非 B 催化剂则观察到持续递减。与非 B 催化剂相比，B-(75Ni-25Co)/MA 的碳沉积极低（~3.6 倍）。此外，密度泛函理论研究还表明，在B 的存在下，75Ni25Co 不同位点的碳吸附能 ( E _{ads ) 显着降低了 ~0.5 eV，从而阻碍了碳在表面上的形成。}

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NaBH4-Assisted Synthesis of B–(Ni–Co)/MgAl2O4 Nanostructures for the Catalytic Dry Reforming of Methane

Carbon deposition on a catalyst surface is detrimental to the dry reforming of methane (DRM) reaction. The addition of boron (B) is found to be effective in lowering carbon deposition. In this study, bimetallic Ni, Co catalysts over MgAl₂O₄(MA) [B–(Ni–Co)/MA] with different Ni/Co ratios are synthesized by the NaBH₄ reduction method and examined for DRM at 600 °C and atmospheric pressure. The NaBH₄ plays crucial roles in reducing metal salt to metal, incorporating B, and enhancing the dispersion of active metallic species in a one-step catalyst preparation method. Rod-like Ni–Co alloy and B–(Ni–Co) nanostructures on the two-dimensional flakes of MA are observed. The Ni-rich B-containing bimetallic [B–(75Ni–25Co)] catalyst exhibits better methane and carbon dioxide conversions compared to other prepared catalysts. The turnover frequency (CH₄) and produced syngas ratio of the B-catalyst are 1.5 and 1.04 times, respectively, higher than the non-B catalyst prepared by the traditional impregnation method with the same Ni/Co ratio. The catalyst [B–(75Ni–25Co)] exhibits higher activity and almost a steady conversion rate, while continuous decrement is observed for the non-B catalyst. Exceptionally low carbon deposition (∼3.6 times) was observed for B–(75Ni–25Co)/MA than the non-B catalyst. Furthermore, the density functional theory investigation also revealed that the adsorption energy (E_ads) of carbon at various sites of 75Ni25Co significantly reduces by ∼0.5 eV in the presence of B, causing hindrance to the formation of carbon over the surface.

更新日期：2022-07-19

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