Artificial Intelligence and High-Throughput Computational Workflows Empowering the Fast Screening of Metal-Organic Frameworks for Hydrogen Storage.

Metal-organic frameworks (MOFs) are one of the most promising hydrogen-storing materials due to their rich specific surface area, adjustable topological and pore structures, and modified functional groups. In this work, we developed automatically parallel computational workflows for high-throughput screening of ∼11,600 MOFs from the CoRE database and discovered 69 top-performing MOF candidates with work capacity greater than 1.00 wt % at 298.5 K and a pressure swing between 100 and 0.1 bar, which is at least twice that of MOF-5. In particular, ZITRUP, OQFAJ01, WANHOL, and VATYIZ showed excellent hydrogen storage performance of 4.48, 3.16, 2.19, and 2.16 wt %. We specifically analyzed the relationship between pore-limiting diameter, largest cavity diameter, void fraction, open metal sites, metal elements or nonmetallic atomic elements, and deliverable capacity and found that not only geometrical and physical features of crystalline but also chemical properties of adsorbate sites determined the H2 storage capacity of MOFs at room temperature. It is highlighted that we first proposed the modified crystal graph convolutional neural networks by incorporating the obtained geometrical and physical features into the convolutional high-dimensional feature vectors of period crystal structures for predicting H2 storage performance, which can improve the prediction accuracy of the neural network from the former mean absolute error (MAE) of 0.064 wt % to the current MAE of 0.047 wt % and shorten the consuming time to about 10-4 times of high-throughput computational screening. This work opens a new avenue toward high-throughput screening of MOFs for H2 adsorption capacity, which can be extended for the screening and discovery of other functional materials.

Optimizing the electronic structure of CoNx via coupling with N-doped carbon for efficient electrochemical hydrogen evolution.

Transition metal nitrides (TMNs) have been regarded as an excellent class of electrocatalysts for hydrogen evolution reaction (HER), but there is still huge room for improvement. In this work, cobalt nitride (CoNx) coupled with N-doped carbon (NC) and supported by nickel foam (NF) is designed as an efficient HER electrocatalyst (NF/CoNx@NC). The introduction of NC can not only optimize the electronic structure of CoNx to boost the intrinsic activity, but also enhance the electronic conductivity and stability of the catalyst. As a result, NF/CoNx@NC exhibits excellent HER performance. On the one hand, it only needs an overpotential of 69 mV to deliver a current density of 20 mA cm-2 in 1.0 mol/L KOH, far better than that of CoNx (182 mV). On the other hand, the electronic conductivity and stability of the catalyst can be significantly enhanced after the introduction of NC. This work has done successful material design with the goal of enhancing the intrinsic activity, electronic conductivity, and stability, which has certain reference and guiding significance for the design of novel transition metal-based electrocatalysts.

Three-Dimensional Transition Metal Phosphide Heteronanorods for Efficient Overall Water Splitting.

The development of low-cost electrocatalysts with excellent activity and durability for both the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) poses a huge challenge in water splitting. In this study, a simple and scalable strategy is proposed to fabricate 3 D heteronanorods on nickel foam, in which nickel molybdenum phosphide nanorods are covered with cobalt iron phosphide (P-NM-CF HNRs). As a result of the rational design, the P-NM-CF HNRs have a large surface area, tightly connected interfaces, optimized electronic structures, and synergy between the metal atoms. Accordingly, the P-NM-CF HNRs exhibit a remarkably high catalytic activity for the OER under alkaline conditions and wide-pH HER. For overall water splitting, the catalyst only requires a voltage of 1.53 V to reach a current density of 10 mA cm-2 in 1 m KOH with prominent stability, and the activity is not degraded after stability testing for 36 h. This new strategy can inspire the design of durable nonprecious-metal catalysts for large-scale industrial water splitting.

Ternary NiFeZr layered double hydroxides: a highly efficient catalyst for the oxygen evolution reaction.

Transition metal layered double hydroxides (LDHs) have attracted wide public attention as highly promising non-precious metal electrocatalysts. Herein a ternary NiFeZr LDH was reported with excellent OER catalytic activity, benefiting from the rapid charge transfer caused by the synergistic effect of the doping of Zr and three-dimensional nanosheet structures.