Platinum-based catalysts have been considered the most effective electrocatalysts for the hydrogen evolution reaction in water splitting. However, platinum utilization in these electrocatalysts is extremely low, as the active sites are only located on the surface of the catalyst particles. Downsizing catalyst nanoparticles to single atoms is highly desirable to maximize their efficiency by utilizing nearly all platinum atoms. Here we report on a practical synthesis method to produce isolated single platinum atoms and clusters using the atomic layer deposition technique. The single platinum atom catalysts are investigated for the hydrogen evolution reaction, where they exhibit significantly enhanced catalytic activity (up to 37 times) and high stability in comparison with the state-of-the-art commercial platinum/carbon catalysts. The X-ray absorption fine structure and density functional theory analyses indicate that the partially unoccupied density of states of the platinum atoms' 5d orbitals on the nitrogen-doped graphene are responsible for the excellent performance. S ecuring renewable and reliable sources of clean energy is one of the world's foremost challenges. Addressing this challenge is not only critical for the global economy but will also aid in the mitigation of environmental and health hazards caused by fossil fuels 1 . Hydrogen is the cleanest fuel available and is believed to be one of the most promising energy sources of the twenty-first century 2,3 . However, the majority of the hydrogen produced today is derived from steam-reformed methane, which is sourced from fossil reserves and produces a substantial amount of CO 2 (ref. 4). The production of hydrogen from water electrolysis is a promising alternative to the current CO 2 -emitting fossil fuel-based energy systems 5,6 .Platinum (Pt)-based catalysts are generally considered to be the most effective electrocatalysts for the hydrogen evolution reaction (HER) 5,7 . Unfortunately, Pt is expensive and scarce, limiting the commercial potential for such catalysts. The development of active, stable and inexpensive electrocatalysts for water splitting is a key step in the realization of a hydrogen economy, which is based on the use of molecular hydrogen for energy storage.Significant effort has been devoted to the search of non-preciousmetal-based HER catalysts, including sulfide-based materials 8-11 , and C 3 N 4 (refs 12-14). Although these candidate materials show promising activities for the HER, the activities of these catalysts in their present form are insufficient for industrial applications 15 .To overcome the challenges associated with the Pt HER catalysts and to drive the cost of H 2 production from water electrolysis down, it is very important to markedly decrease the Pt loading and increase the Pt utilization efficiency. Currently, supported Pt nanoparticles (NPs) are typically used to promote Pt activity towards the HER. Unfortunately, the geometry of the NPs limit the majority of the Pt atoms to the particle core, deeming them ineffect...
Platinum-nanoparticle-based catalysts are widely used in many important chemical processes and automobile industries. Downsizing catalyst nanoparticles to single atoms is highly desirable to maximize their use efficiency, however, very challenging. Here we report a practical synthesis for isolated single Pt atoms anchored to graphene nanosheet using the atomic layer deposition (ALD) technique. ALD offers the capability of precise control of catalyst size span from single atom, subnanometer cluster to nanoparticle. The single-atom catalysts exhibit significantly improved catalytic activity (up to 10 times) over that of the state-of-the-art commercial Pt/C catalyst. X-ray absorption fine structure (XAFS) analyses reveal that the low-coordination and partially unoccupied densities of states of 5d orbital of Pt atoms are responsible for the excellent performance. This work is anticipated to form the basis for the exploration of a next generation of highly efficient single-atom catalysts for various applications.
Ambient-air-stable Li3InCl6 halide solid electrolyte, with high ionic conductivity of 1.49 × 10−3 S cm−1 at 25 °C, delivers essential advantages over commercial sulfide-based solid electrolyte.
Single atom catalysts exhibit particularly high catalytic activities in contrast to regular nanomaterial-based catalysts. Until recently, research has been mostly focused on single atom catalysts, and it remains a great challenge to synthesize bimetallic dimer structures. Herein, we successfully prepare high-quality one-to-one A-B bimetallic dimer structures (Pt-Ru dimers) through an atomic layer deposition (ALD) process. The Pt-Ru dimers show much higher hydrogen evolution activity (more than 50 times) and excellent stability compared to commercial Pt/C catalysts. X-ray absorption spectroscopy indicates that the Pt-Ru dimers structure model contains one Pt-Ru bonding configuration. First principle calculations reveal that the Pt-Ru dimer generates a synergy effect by modulating the electronic structure, which results in the enhanced hydrogen evolution activity. This work paves the way for the rational design of bimetallic dimers with good activity and stability, which have a great potential to be applied in various catalytic reactions.
As one of the most promising negative electrode materials in lithium‐ion batteries (LIBs), SnO2 experiences intense investigation due to its high specific capacity and energy density, relative to conventional graphite anodes. In this study, for the first time, atomic layer deposition (ALD) is used to deposit SnO2, containing both amorphous and crystalline phases, onto graphene nanosheets (GNS) as anodes for LIBs. The resultant SnO2‐graphene nanocomposites exhibit a sandwich structure, and, when cycled against a lithium counter electrode, demonstrate a promising electrochemical performance. It is demonstrated that the introduction of GNS into the nanocomposites is beneficial for the anodes by increasing their electrical conductivity and releasing strain energy: thus, the nanocomposite electrode materials maintain a high electrical conductivity and flexibility. It is found that the amorphous SnO2‐GNS is more effective than the crystalline SnO2‐GNS in overcoming electrochemical and mechanical degradation; this observation is consistent with the intrinsically isotropic nature of the amorphous SnO2, which can mitigate the large volume changes associated with charge/discharge processes. It is observed that after 150 charge/discharge cycles, 793 mA h g−1 is achieved. Moreover, a higher coulombic efficiency is obtained for the amorphous SnO2‐GNS composite anode. This study provides an approach to fabricate novel anode materials and clarifies the influence of SnO2 phases on the electrochemical performance of LIBs.
To promote the development of solid‐state batteries, polymer‐, oxide‐, and sulfide‐based solid‐state electrolytes (SSEs) have been extensively investigated. However, the disadvantages of these SSEs, such as high‐temperature sintering of oxides, air instability of sulfides, and narrow electrochemical windows of polymers electrolytes, significantly hinder their practical application. Therefore, developing SSEs that have a high ionic conductivity (>10−3 S cm−1), good air stability, wide electrochemical window, excellent electrode interface stability, low‐cost mass production is required. Herein we report a halide Li+ superionic conductor, Li3InCl6, that can be synthesized in water. Most importantly, the as‐synthesized Li3InCl6 shows a high ionic conductivity of 2.04×10−3 S cm−1 at 25 °C. Furthermore, the ionic conductivity can be recovered after dissolution in water. Combined with a LiNi0.8Co0.1Mn0.1O2 cathode, the solid‐state Li battery shows good cycling stability.
A highly lithium ionic conductive solid-state electrolyte coating layer significantly increases cathode performance in lithium ion batteries.
The electrochemical reduction of carbon dioxide (CO 2 RR) offers a compelling route to energy storage and high-value chemical manufacture. The presence of sulfur atoms in catalyst surfaces promotes undercoordinated sites, thereby improving the electrochemical reduction of CO 2 to formate. The resulting sulfurmodulated tin catalysts accelerate CO 2 RR at geometric current densities of 55 mA cm À2 at À0.75 V versus RHE with a Faradaic efficiency of 93%.
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