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.

The main challenge associated with sodium-ion battery (SIB) anodes is a search for novel candidate materials with high capacity and excellent rate capability. The most commonly used and effective route for graphene-based anode design is the introduction of in-plane “hole” defects via nitrogen-doping; this creates a spacious reservoir for storing more energy. Inspired by mountains in nature, herein, we propose another way – the introduction of blistering in graphene instead of making “holes”; this facilitates adsorbing/inserting more Na⁺ ions. In order to properly answer the key question: ““protrusions” or “holes” in graphene, which is better for sodium ion storage?”, two types of anode materials with a similar doping level were designed: a phosphorus-doped graphene (GP, with protrusions) and a nitrogen-doped graphene (GN, with holes). As compared with GN, the GP anode perfectly satisfies all the desired criteria: it reveals an ultrahigh capacity (374 mA h g⁻¹ after 120 cycles at 25 mA g⁻¹) comparable to the best graphite anodes in a standard Li-ion battery (∼372 mA h g⁻¹), and exhibits an excellent rate capability (210 mA h g⁻¹ at 500 mA g⁻¹). In situ transmission electron microscopy (TEM) experiments and density functional theory (DFT) calculations were utilized to uncover the origin of the enhanced electrochemical activity of “protrusions” compared to “holes” in SIBs, down to the atomic scale. The introduction of protrusions through P-doping into graphene is envisaged to be a novel effective way to enhance the capacity and rate performance of SIBs.

Ni²⁺Mn³⁺ layered double hydroxide (LDH) nanoplatelets have been hydrothermally synthesized in a homogeneous precipitation of mixed Ni²⁺/Mn²⁺ salts at a molar ratio of 2 : 1 via the hydrolysis of hexamethylenetetramine (HMT) and in situ oxidation with H₂O₂. After anion-exchange, NiMn LDH was exfoliated into unilamellar nanosheets. Subsequent flocculation of NiMn LDH nanosheets with (reduced) graphene oxide (GO/rGO) into superlattice composites was achieved and further tested as electrocatalysts for oxygen evolution reaction (OER). The face-to-face heteroassembly of NiMn LDH nanosheets with conductive rGO at an alternating sequence resulted in a small overpotential of 0.26 V and a Tafel slope of 46 mV per decade, which is much superior to as-exfoliated nanosheets. The analyses of electrochemical activity surface area (ECSA) and impedance spectra clearly indicated that the superlattice structure was ideal in facilitating the migration/transfer of the charge and reactants, revealing the electrochemical energetics and mechanism behind the synergistic effect arising from molecular hybridization. The proof of concept toward total water splitting using the newly developed hybrid electrocatalyst was demonstrated by an electrolysis cell powered by a single AA battery.