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Decoupling Strategy for Enhanced Syngas Generation from Photoelectrochemical CO2 Reduction

机译:从光电化学二氧化碳减少中产生增强合成气的去耦策略

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摘要

Photoelectrochemical CO reduction into syngas (a mixture of CO and H ) provides a promising route to mitigate greenhouse gas emissions and store intermittent solar energy into value-added chemicals. Design of photoelectrode with high energy conversion efficiency and controllable syngas composition is of central importance but remains challenging. Herein, we report a decoupling strategy using dual cocatalysts to tackle the challenge based on joint computational and experimental investigations. Density functional theory calculations indicate the optimization of syngas generation using a combination of fundamentally distinctive catalytic sites. Experimentally, by integrating spatially separated dual cocatalysts of a CO-generating catalyst and a H -generating catalyst with GaN nanowires on planar Si photocathode, we report a record high applied bias photon-to-current efficiency of 1.88% and controllable syngas products with tunable CO/H ratios (0–10) under one-sun illumination. Moreover, unassisted solar CO reduction with a solar-to-syngas efficiency of 0.63% is demonstrated in a tandem photoelectrochemical cell.
机译:光电化学CO还原到合成气(CO和H的混合物)提供了一个有望的途径,以减轻温室气体排放,并将间歇太阳能存储成增值化学品。具有高能量转换效率和可控合成气组成的光电系数具有核心重要性,但仍然具有挑战性。在此,我们通过双助催化剂报告了解耦策略,以基于联合计算和实验研究来解决挑战。密度函数理论计算表明使用基本上独特的催化位点的组合来优化合成气的优化。通过在平面Si光电阴极上将共同产生催化剂的空间分离的双助催化剂与GaN纳米线相容,通过可调谐,通过GaN纳米线与GaN纳米线与GaN纳米线一起报告1.88%和可控制的合成气产品的记录高施加的偏置光子至电流效率单阳照明下的CO / H比率(0-10)。此外,在串联光电化细胞中证明了具有0.63%的太阳能到合成气效率的无统一的太阳能CO。

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