Increasing CO2 concentration in the atmosphere is believed to have a profound impact on the global climate. To reverse the impact would necessitate not only curbing the reliance on fossil fuels but also developing effective strategies capture and utilize CO2 from the atmosphere. Among several available strategies, CO2 reduction via the electrochemical or photochemical approach is particularly attractive since the required energy input can be potentially supplied from renewable sources such as solar energy. In this Review, an overview on these two different but inherently connected approaches is provided and recent progress on the development, engineering, and understanding of CO2 reduction electrocatalysts and photocatalysts is summarized. First, the basic principles that govern electrocatalytic or photocatalytic CO2 reduction and their important performance metrics are discussed. Then, a detailed discussion on different CO2 reduction electrocatalysts and photocatalysts as well as their generally designing strategies is provided. At the end of this Review, perspectives on the opportunities and possible directions for future development of this field are presented.

Electrocatalytic carbon dioxide reduction to formate is desirable but challenging. Current attention is mostly focused on tin-based materials, which, unfortunately, often suffer from limited Faradaic efficiency. The potential of bismuth in carbon dioxide reduction has been suggested but remained understudied. Here, we report that ultrathin bismuth nanosheets are prepared from the in situ topotactic transformation of bismuth oxyiodide nanosheets. They process single crystallinity and enlarged surface areas. Such an advantageous nanostructure affords the material with excellent electrocatalytic performance for carbon dioxide reduction to formate. High selectivity (~100%) and large current density are measured over a broad potential, as well as excellent durability for >10 h. Its selectivity for formate is also understood by density functional theory calculations. In addition, bismuth nanosheets were coupled with an iridium-based oxygen evolution electrocatalyst to achieve efficient full-cell electrolysis. When powered by two AA-size alkaline batteries, the full cell exhibits impressive Faradaic efficiency and electricity-to-formate conversion efficiency.

Reversible electrochemical storage of alkali metal ions is the basis of many secondary batteries. Over years, various electrode materials are developed and optimized for a specific type of alkali metal ions (Li , Na , or K ), yet there are very few (if not none) candidates that can serve as a universal host material for all of them. Herein, a facile solvothermal method is developed to prepare VS nanosheet assemblies. Individual nanosheets are featured with a few atomic layer thickness, and they are hierarchically arranged with minimized stacking. Electrochemical measurements show that VS nanosheet assemblies enable the rapid and durable storage of Li , Na , or K ions. Most remarkably, the large reversible specific capacity and great cycling stability observed for both Na and K are extraordinary and superior to most existing electrode materials. The experimental results of this study are further supported by density functional theory calculations showing that the layered structure of VS has large adsorption energy and low diffusion barriers for the intercalation of alkali metal ions.

All‐solid‐state lithium batteries (ASSLBs) are considered as the next generation electrochemical energy storage devices because of their high safety and energy density, simple packaging, and wide operable temperature range. The critical component in ASSLBs is the solid‐state electrolyte. Among all solid‐state electrolytes, the sulfide electrolytes have the highest ionic conductivity and favorable interface compatibility with sulfur‐based cathodes. The ionic conductivity of sulfide electrolytes is comparable with or even higher than that of the commercial organic liquid electrolytes. However, several critical challenges for sulfide electrolytes still remain to be solved, including their narrow electrochemical stability window, the unstable interface between the electrolyte and the electrodes, as well as lithium dendrite formation in the electrolytes. Herein, the emerging sulfide electrolytes and preparation methods are reviewed. In particular, the required properties of the sulfide electrolytes, such as the electrochemical stabilities of the electrolytes and the compatible electrode/electrolyte interfaces are highlighted. The opportunities for sulfide‐based ASSLBs are also discussed.

A simple and scalable method is developed to synthesize TiO(2)/graphene nanostructured composites as high-performance anode materials for Li-ion batteries using hydroxyl titanium oxalate (HTO) as the intermediate for TiO(2). With assistance of a surfactant, amorphous HTO can condense as a flower-like nanostructure on graphene oxide (GO) sheets. By calcination, the HTO/GO nanocomposite can be converted to TiO(2)/graphene nanocomposite with well preserved flower-like nanostructure. In the composite, TiO(2) nanoparticles with an ultrasmall size of several nanometers construct the porous flower-like nanostructure which strongly attached onto conductive graphene nanosheets. The TiO(2)/graphene nanocomposite is able to deliver a capacity of 230 mA h g(-1) at 0.1 C (corresponding to a current density of 17 mA g(-1)), and demonstrates superior high-rate charge-discharge capability and cycling stability at charge/discharge rates up to 50 C in a half cell configuration. Full cell measurement using the TiO(2)/graphene as the anode material and spinel LiMnO(2) as the cathode material exhibit good high-rate performance and cycling stability, indicating that the TiO(2)/graphene nanocomposite has a practical application potential in advanced Li-ion batteries.

The conversion of CO 2 to value-added products using electrical or solar energy represents an attractive means for the capture and utilization of atmospheric CO 2 . Formate is a popular product from CO 2 reduction, but its reaction selectivity is usually unsatisfactory. Tin-based materials have attracted most attention for formate production at present. Unfortunately, most of them only exhibit moderate selectivity in a narrow and highly cathodic potential window. In this study, we demonstrate that traditionally under-explored bismuth has a much greater potential for formate production than tin or other materials. Mesoporous bismuth nanosheets are prepared here by the cathodic transformation of atomic-thick bismuth oxycarbonate nanosheets. They enable the selective CO 2 reduction to formate with large current density, excellent Faradaic efficiency (~100%) over a broad potential window and great operation stability. Moreover, we integrate Bi nanosheets with an oxygen evolution reaction electrocatalyst in full cells, and achieve efficient and robust solar conversion of CO 2 /H 2 O to formate/O 2 .

The introduction of protrusions through P-doping into graphene is an effective strategy to enhance electrochemical performances in SIBs.

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