S-Scheme Co9S8@Cd0.8Zn0.2S-DETA Hierarchical Nanocages Bearing Organic CO2 Activators for Photocatalytic Syngas Production,Advanced Energy Materials

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S-Scheme Co9S8@Cd0.8Zn0.2S-DETA Hierarchical Nanocages Bearing Organic CO2 Activators for Photocatalytic Syngas Production
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2023-03-01 , DOI: 10.1002/aenm.202203290
Bo Su ₁ , Mei Zheng ₁ , Wei Lin ₁ , Xue Feng Lu ₁ , Deyan Luan ₂ , Sibo Wang ₁ , Xiong Wen (David) Lou ₃

Affiliation

Delicate modulations of CO₂ activation and charge carrier separation/migration are challenging, yet imperative to augment CO₂ photoreduction efficiency. Herein, by supporting diethylenetriamine (DETA)-functionalized Cd_0.8Zn_0.2S nanowires on the exterior surface of hollow Co₉S₈ polyhedrons, hierarchical Co₉S₈@Cd_0.8Zn_0.2S-DETA nanocages are fabricated as an S-scheme photocatalyst for reducing CO₂ and protons to produce syngas (CO and H₂). The amine groups strengthen adsorption and activation of CO₂, while the “nanowire-on-nanocage” hierarchical hollow heterostructure with an S-scheme interface boosts separation and transfer of photoinduced charges. Employing Co(bpy)₃²⁺ as a cocatalyst, the optimal photocatalyst effectively produces CO and H₂ in rates of 70.6 and 18.6 µmol h⁻¹ (i.e., 4673 and 1240 µmol g⁻¹ h⁻¹), respectively, affording an apparent quantum efficiency of 9.45% at 420 nm, which is the highest value under comparable conditions. Ultraviolet photoelectron spectroscopy, Kelvin probe, and electron spin resonance confirm the S-schematic charge-transfer process in the photocatalyst. The key COOH^* species responsible for CO₂-to-CO reduction is detected by in-situ diffuse reflectance infrared Fourier transform spectroscopy and endorsed by density functional theory calculations, and thus a possible CO₂ reduction mechanism is proposed.

中文翻译：

S-方案 Co9S8@Cd0.8Zn0.2S-DETA 分层纳米笼承载有机 CO2 活化剂用于光催化合成气生产

CO ₂活化和载流子分离/迁移的精细调节具有挑战性，但对于提高CO ₂光还原效率是必不可少的。在此，通过将二乙烯三胺 (DETA) 功能化的 Cd _0.8 Zn _{0.2 S 纳米线负载在中空 Co}₉ S ₈多面体的外表面上，分级 Co ₉ S ₈ @Cd _0.8 Zn _0.2 S-DETA 纳米笼被制造为 S 型光催化剂用于还原 CO ₂和质子以产生合成气（CO 和 H ₂）。胺基加强了对CO _{2的吸附和活化}，而具有 S 型界面的“纳米笼上纳米线”分层空心异质结构促进了光生电荷的分离和转移。使用 Co(bpy) ₃²⁺作为助催化剂，最佳光催化剂有效地产生 CO 和 H ₂的速率分别为 70.6 和 18.6 µmol h ⁻¹（即，4673 和 1240 µmol g ⁻¹ h ⁻¹），提供在 420 nm 处的表观量子效率为 9.45%，这是可比条件下的最高值。紫外光电子能谱、开尔文探针和电子自旋共振证实了光催化剂中的 S-示意图电荷转移过程。产生 CO ₂的关键 COOH ^*物质通过原位漫反射红外傅里叶变换光谱检测到-to-CO 还原，并通过密度泛函理论计算得到证实，因此提出了一种可能的CO _{2还原机制。}

更新日期：2023-03-01

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