The development of an effective one‐photon excitation pathway to improve the charge‐carrier separation and mobility of semiconductors, which have been proven to be favorable for heterogeneous catalysis, is highly desirable but remains a great challenge. Herein, a high‐throughput one‐photon excitation pathway is reported by constructing 0D carbon dots/3D porous carbon nitride nanovesicles (denoted as CDs/PCN NVs) heterostructures for photocatalytic hydrogen evolution. In particular, the optimum CDs/PCN NVs heterostructures exhibit an impressive performance of 14.022 mmol h−1 g−1, which is 56.54 times higher than that of pristine CN. Detailed characterization reveals that the improved performance is primarily attributed to the high‐throughput and one‐photon excitation pathway. The former could be attributed to a great deal of CDs with high charge‐carrier mobility coupled to PCN NVs, which enable more electrons to be photoexcited via the broad absorption response, and the multiple reflection of incident light owing to the porous nanovesicle structure with shortened route of carriers migrating toward the surface; the latter would lead to the photoinduced holes and electrons accumulated at the valence band of PCN NVs and surface of CDs, respectively, achieving an effective spatial separation. The high‐throughput one‐photon excitation pathway demonstrated here may provide insights into the development of nanocomposites for various related applications.

Size-dependent surface energy associated with atomic number N, γ(N), of Ag quasicrystal clusters was investigated using density functional theory and broken-bond theory. It is found that the value of γ(N) is 0.55-0.66 eV/atom, similar to the value of their counterparts in bulk. This is due to the increase of cohesive energy E c (N) and the decrease of surface coordinate number associated with the decreasing of N. As N decreases, the partial density of states shifts to higher binding energy, and there is electronic charge transfer from the sp band into the d band, which leads to the increase of cohesive energy.

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Carbon nanofibers films are typical flexible electrode in the field of energy storage, but their application in Zinc-ion hybrid capacitors (ZIHCs) is limited by the low energy density due to the lack of active adsorption sites. In this work, an in-situ exfoliation strategy is reported to modulate the chemisorption sites of carbon nanofibers by high pyridine/pyrrole nitrogen doping and carbonyl functionalization. The experimental results and theoretical calculations indicate that the highly electronegative pyridine/pyrrole nitrogen dopants can not only greatly reduce the binding energy between carbonyl group and Zn2+ by inducing charge delocalization of the carbonyl group, but also promote the adsorption of Zn2+ by bonding with the carbonyl group to form N–Zn–O bond. Benefit from the multiple highly active chemisorption sites generated by the synergy between carbonyl groups and pyridine/pyrrole nitrogen atoms, the resulting carbon nanofibers film cathode displays a high energy density, an ultralong-term lifespan, and excellent capacity reservation under commercial mass loading (14.45 mg cm‒2). Particularly, the cathodes can also operate stably in flexible or quasi-solid devices, indicating its application potential in flexible electronic products. This work established a universal method to solve the bottleneck problem of insufficient active adsorption sites of carbon-based ZIHCs.Imoproved should be changed into Improved.

The heart of current high-throughput computational design for two-dimensional (2D) van der Waals (vdW) functional heterostructures is Anderson's rule (AR). This non-interacting model, however, inevitably introduces error and uncertainty in design results, problems which remain neglected. We report that, even for a non-magnetic system, the current high-throughput design framework commonly omits potential candidates in specific fields, such as heterostructure solar cell research. Therefore, this framework is fragile to extend to all subfields of functional vdW heterostructures. Through the analysis of several factors, such fragility is found to arise mainly from interlayer orbital coupling. This effect is omitted by AR and causes statistical deviation in the prediction of electronic properties. In the absence of a more advanced and universal physical model for describing interlayer orbital coupling, we propose a robust high-throughput design framework to reduce the omission of potential candidates. This work deepens the understanding of high-throughput design for 2D vdW functional heterostructures and provides insight into their development.