Material design is one of the major driving forces to enhance the intrinsic light harvesting ability of a photocatalyst. Herein, the design of black TiO2−x/CuxO with chiral‐like structures where Pt single atom (SA) is successfully deposited on both black TiO2−x and CuxO for visible‐light H2 generation is reported. Pt is well dispersed not only in the TiO2−x surface but also at the surface of CuxO, forming single‐atom alloys. Oxygen defects stabilize the Pt SAs deposition, which significantly enlarge the space charge layer, facilitating both the separation and transfer of photogenerated charge carriers. This structural optimization endows the black TiO2−x/CuxO/Pt film excellent light harvesting ability in the visible region, making it a promising visible‐light‐responsive photocatalyst. This work is expected to provide insights into the rational construction of nanostructured materials with chiral nematic structure exhibiting improved light harvesting ability.

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The configuration and geometry of chemical reactors underpins the accuracy of performance evaluation for photocatalytic materials and, accordingly, the development and validation of thermodynamic and kinetic model reactions. The lack of accurate photonic, mass, and heat transport profiles for photochemical reactors hinder standardization, scale-up, and ultimately comparison between different experiments. This work proposes two contributions at the interface between engineering of chemical process and materials science: (A) an automated compact stainless-steel photoreactor with 40 cm3 and 65 cm2 of volume and area, respectively, for hydrogen photoproduction as a model reaction and (B) the synthesis, characterization, and performance of TiO2 Schottky junctions, using Pd, Pt, or Au nanoparticles (ca. 0.5, 1, 2wt.% loadings each) to validate the operation of the reactor. A photonic profile methodology is implemented to the studied reactor to obtain the local light absorption profile, opening up for evaluation of the local quantum yield calculation for the selected materials. A combination of transmission electron microscopy, (X-ray/ultraviolet) photoelectron/electron, energy loss/infrared spectroscopies, X-ray scattering, inductively coupled plasma atomic emission spectroscopy, and ultraviolet-visible spectrophotometry is employed to determine the distinctive surface and bulk properties to build structure-function correlations. The (Pd, Pt, Au)/TiO2 Schottky junction exhibits H2 production rates slightly higher than previous studies, with quantum yields almost 2-fold higher than reported values. These results, demonstrate that the proposed novel geometry of the photoreactor improves the photonic, heat, and mass profiles. An in-depth analysis of the Au plasmon was investigated coupling electron energy loss spectroscopy, UV-vis, and transmission electron microscope, resulting in insightful information about the Au NP mode at the TiO2 interface.