Unveiling the critical role of TiO2-supported atomically dispersed Cu species for enhanced photofixation of N2 to nitrate

IF 6.2 3区 综合性期刊 Q1 Multidisciplinary
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引用次数: 0

Abstract

Nitrate products are widely used in manufacturing as crucial raw materials and fertilizers. The traditional nitrate synthesis process involves high energy consumption and emission, thereby opposing the goals of zero-carbon emission and green chemistry. Thus, a sustainable roadmap for nitrate synthesis that uses green energy input, clean N sources, and direct catalytic processes is urgently required (e.g., developing a novel photosynthesis system). Here, we synthesized TiO2-supported atomically dispersed Cu species for N2 photofixation to nitrate in a flow reactor. The optimized photocatalyst yielded a high nitrate photosynthesis rate of 0.93 μmol h−1 and selectivity of ∼90%, which is superior to most of the values reported thus far. Further, experimental results and in-situ investigations revealed that the atomically dispersed Cu sites in the as-designed sample significantly enhanced the separation and transfer efficiency of photogenerated carriers, adsorption and activation of reactants, and the formation of chemisorbed NOx intermediates, thereby realizing the excellent photofixation of N2 to nitrate.

揭示TiO2支持的原子分散Cu物种在增强N2对硝酸盐的光固定中的关键作用
硝酸盐产品作为重要的原材料和肥料被广泛应用于制造业。传统的硝酸盐合成工艺能耗高、排放量大,与零碳排放和绿色化学的目标背道而驰。因此,利用绿色能源输入、清洁氮源和直接催化工艺(如开发新型光合作用系统)的可持续硝酸盐合成路线图亟待开发。在此,我们合成了二氧化钛(TiO2)支撑的原子分散铜物种,用于在流动反应器中将 N2 光固化为硝酸盐。优化后的光催化剂硝酸盐光合作用率高达 0.93 μmol h-1,选择性高达 90%,优于目前报道的大多数数值。此外,实验结果和原位研究表明,设计样品中原子分散的铜位点显著提高了光生载流子的分离和转移效率、反应物的吸附和活化以及化学吸附 NOx 中间产物的形成,从而实现了 N2 到硝酸盐的良好光固化。
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来源期刊
Fundamental Research
Fundamental Research Multidisciplinary-Multidisciplinary
CiteScore
4.00
自引率
1.60%
发文量
294
审稿时长
79 days
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