Electrochemical carbon dioxide reduction reaction (CO2RR) offers a promising way of effectively converting CO2 to value‐added chemicals and fuels by utilizing renewable electricity. To date, the electrochemical reduction of CO2 to single‐carbon products, especially carbon monoxide and formate, has been well achieved. However, the efficient conversion of CO2 to more valuable multicarbon products (e.g., ethylene, ethanol, n‐propanol, and n‐butanol) is difficult and still under intense investigation. Here, recent progresses in the electrochemical CO2 reduction to multicarbon products using copper‐based catalysts are reviewed. First, the mechanism of CO2RR is briefly described. Then, representative approaches of catalyst engineering are introduced toward the formation of multicarbon products in CO2RR, such as composition, morphology, crystal phase, facet, defect, strain, and surface and interface. Subsequently, key aspects of cell engineering for CO2RR, including electrode, electrolyte, and cell design, are also discussed. Finally, recent advances are summarized and some personal perspectives in this research direction are provided.
Electrocatalytic carbon dioxide reduction reaction (CO2RR) holds significant potential to promote carbon neutrality. However, the selectivity toward multicarbon products in CO2RR is still too low to meet practical applications. Here the authors report the delicate synthesis of three kinds of Ag–Cu Janus nanostructures with {100} facets (JNS‐100) for highly selective tandem electrocatalytic reduction of CO2 to multicarbon products. By controlling the surfactant and reduction kinetics of Cu precursor, the confined growth of Cu with {100} facets on one of the six equal faces of Ag nanocubes is realized. Compared with Cu nanocubes, Ag65–Cu35 JNS‐100 demonstrates much superior selectivity for both ethylene and multicarbon products in CO2RR at less negative potentials. Density functional theory calculations reveal that the compensating electronic structure and carbon monoxide spillover in Ag65–Cu35 JNS‐100 contribute to the enhanced CO2RR performance. This study provides an effective strategy to design advanced tandem catalysts toward the extensive application of CO2RR.
Given the high energy density and eco-friendly characteristics, lithium-carbon dioxide (Li-CO
2
) batteries have been considered to be a next-generation energy technology to promote carbon neutral and space exploration. However, Li-CO
2
batteries suffer from sluggish reaction kinetics, causing large overpotential and poor energy efficiency. Here, we observe enhanced reaction kinetics in aprotic Li-CO
2
batteries with unconventional phase 4H/face-centered cubic (fcc) iridium (Ir) nanostructures grown on gold template. Significantly, 4H/fcc Ir exhibits superior electrochemical performance over fcc Ir in facilitating the round-trip reaction kinetics of Li
+
-mediated CO
2
reduction and evolution, achieving a low charge plateau below 3.61 V and high energy efficiency of 83.8%. Ex situ/in situ studies and theoretical calculations reveal that the boosted reaction kinetics arises from the highly reversible generation of amorphous/low-crystalline discharge products on 4H/fcc Ir via the Ir-O coupling. The demonstration of flexible Li-CO
2
pouch cells with 4H/fcc Ir suggests the feasibility of using unconventional phase nanomaterials in practical scenarios.
Among different CO 2 conversion technologies, electrochemical CO 2 reduction reaction (CO 2 RR) offers a sustainable strategy to convert CO 2 into value-added chemicals and fuels. [5][6][7][8] To promote the practical applications of electrochemical CO 2 RR, great research efforts, such as, composition modulation, [9,10] facet regulation, [11,12] defect control, [13][14][15][16] strain adjustment, [17,18] and phase engineering [19][20][21][22][23] of catalysts, have been devoted to tune the reaction pathway and increase the selectivity of target products. [24] In particular, highly efficient and selective conversion of CO 2 into carbon monoxide (CO) is a promising way toward industrial application as CO can be easily separated and widely utilized as a feedstock to generate various highvalue chemicals and fuels. [25,26] Metal nanomaterials, especially gold (Au) [27][28][29][30] and silver (Ag), [31][32][33] are promising catalysts for the electrochemical reduction of CO 2 to CO. However, most metal catalysts still suffer from low activity and the volcano-type CO Faradaic efficiency (FE) as a function of applied potentials.
Because
of the distinct electronic structures and stable chemical
properties, rhodium materials are one of the most important noble
metal catalysts for various kinds of industrial chemical processes.
Recently, two-dimensional (2D) rhodium nanomaterials have emerged
as excellent catalysts for many essential chemical reactions, such
as hydrogen evolution, oxygen evolution, alcohol oxidation, carbon
monoxide oxidation, hydrogen generation, and organic reactions. In
this Review, we give an overview of recent advances in the controlled
synthesis and catalytic applications of 2D rhodium nanomaterials.
We first introduce the typical synthetic methods of 2D rhodium nanomaterials,
together with the underlying mechanisms. Then, the catalytic applications
of 2D rhodium nanomaterials in representative chemical reactions are
systematically described. Finally, we summarize the recent research
progress and provide some personal perspectives on critical challenges
and future research opportunities in this emerging research direction.
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