skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


Title: Carbon Catalysts for Electrochemical CO 2 Reduction toward Multicarbon Products
Abstract Electrochemical CO2reduction offers a compelling route to mitigate atmospheric CO2concentration and store intermittent renewable energy in chemical bonds. Beyond C1, C2+feedstocks are more desirable due to their higher energy density and more significant market need. However, the CO2‐to‐C2+reduction suffers from significant barriers of CC coupling and complex reaction pathways. Due to remarkable tunability over morphology/pore architecture along with great feasibility of functionalization to modify the electronic and geometric structures, carbon materials, serving as active components, supports, and promoters, provide exciting opportunities to tune both the adsorption properties of intermediates and the local reaction environment for the CO2reduction, offering effective solutions to enable CC coupling and steer C2+evolution. However, general design principles remain ambiguous, causing an impediment to rational catalyst refinement and application thrusts. This review clarifies insightful design principles for advancing carbon materials. First, the current performance status and challenges are discussed and effective strategies are outlined to promote C2+evolution. Further, the correlation between the composition, structure, and morphology of carbon catalysts and their catalytic behavior is elucidated to establish catalytic mechanisms and critical factors determining C2+performance. Finally, future research directions and strategies are envisioned to inspire revolutionary advancements.  more » « less
Award ID(s):
1804326
PAR ID:
10368049
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Energy Materials
Volume:
12
Issue:
24
ISSN:
1614-6832
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; (, Energy & Environmental Science)
    null (Ed.)
    Electrochemical reduction of CO 2 into value-added fuels and chemicals driven by renewable energy presents a potentially sustainable route to mitigate CO 2 emissions and alleviate the dependence on fossil fuels. While tailoring the electronic structure of active components to modulate their intrinsic reactivity could tune the CO 2 reduction reaction (CO 2 RR), their use is limited by the linear scaling relation of intermediates. Due to the high susceptibility of the CO 2 RR to the local CO 2 concentration/pH and mass transportation of CO 2 /intermediates/products near the gas–solid–liquid three-phase interface, engineering catalysts’ morphological and interfacial properties holds great promise to regulate the CO 2 RR, which are irrelevant with linear scaling relation and possess high resistance to harsh reaction conditions. Herein, we provide a comprehensive overview of recent advances in tuning CO 2 reduction electrocatalysis via morphology and interface engineering. The fundamentals of the CO 2 RR and design principles for electrode materials are presented firstly. Then, approaches to build an efficient three-phase interface, tune the surface wettability, and design a favorable morphology are summarized; the relationship between the properties of engineered catalysts and their CO 2 RR performance is highlighted to reveal the activity-determining parameters and underlying catalytic mechanisms. Finally, challenges and opportunities are proposed to suggest the future design of advanced CO 2 RR electrode materials. 
    more » « less
  2. ; ; ; ; (, Advanced Energy Materials)
    Abstract The electrochemical carbon dioxide reduction reaction (CO2RR) is a promising approach for reducing atmospheric carbon dioxide (CO2) emissions, allowing harmful CO2to be converted into more valuable carbon‐based products. On one hand, single carbon (C1) products have been obtained with high efficiency and show great promise for industrial CO2capture. However, multi‐carbon (C2+) products possess high market value and have demonstrated significant promise as potential products for CO2RR. Due to CO2RR's multiple pathways with similar equilibrium potentials, the extended reaction mechanisms necessary to form C2+products continue to reduce the overall selectivity of CO2‐to‐C2+electroconversion. Meanwhile, CO2RR as a whole faces many challenges relating to system optimization, owing to an intolerance for low surface pH, systemic stability and utilization issues, and a competing side reaction in the form of the H2evolution reaction (HER). Ethylene (C2H4) remains incredibly valuable within the chemical industry; however, the current established method for producing ethylene (steam cracking) contributes to the emission of CO2into the atmosphere. Thus, strategies to significantly increase the efficiency of this technology are essential. This review will discuss the vital factors influencing CO2RR in forming C2H4products and summarize the recent advancements in ethylene electrosynthesis. 
    more » « less
  3. ; ; (, ChemCatChem)
    Abstract Hybrid organic‐inorganic heterogeneous catalytic interfaces, where traditional catalytic materials are modified with self‐assembled monolayers (SAMs), create promising features to control a wide range of catalytic processes through the design of dual organic‐inorganic active sites and the induced confinement effect. To provide a fundamental insight, we investigated CO2electroreduction into valuable C2chemicals (CO2RR‐to‐C2) over SAM‐modulated Cu. Our theoretical results show that 1/4 monolayer aminothiolates improve the stability, activity and selectivity of CO2RR‐to‐C2by: (1) decreasing surface energy to suppress surface reconstruction; (2) facilitating CO2activation and C−C coupling through dual organic‐inorganic (i. e., −NH, Cu) active sites; (3) promoting C−C coupling via confinement effects that enlarge the adsorption energy difference between CO*and COH*; (4) inducing local electric fields to Cu surface and changing its dipole moment and polarizability to be in favor of C−C coupling under electrode/electrolyte interfacial electric field. 
    more » « less
  4. ; ; ; ; ; ; ; ; (, Advanced Materials)
    Abstract Carbon nanomaterials are promising metal‐free catalysts for energy conversion and storage, but the catalysts are usually developed via traditional trial‐and‐error methods. To rationally design and accelerate the search for the highly efficient catalysts, it is necessary to establish design principles for the carbon‐based catalysts. Here, theoretical analysis and material design of metal‐free carbon nanomaterials as efficient photo‐/electrocatalysts to facilitate the critical chemical reactions in clean and sustainable energy technologies are reviewed. These reactions include the oxygen reduction reaction in fuel cells, the oxygen evolution reaction in metal–air batteries, the iodine reduction reaction in dye‐sensitized solar cells, the hydrogen evolution reaction in water splitting, and the carbon dioxide reduction in artificial photosynthesis. Basic catalytic principles, computationally guided design approaches and intrinsic descriptors, catalytic material design strategies, and future directions are discussed for the rational design and synthesis of highly efficient carbon‐based catalysts for clean energy technologies. 
    more » « less
  5. ; ; ; (, Small Methods)
    Abstract The development of low‐cost and efficient electrocatalysts for nitrogen reduction reaction (NRR) at ambient conditions is crucial for NH3synthesis and provides an alternative to the traditional Harber‐Bosch process. Herein, by means of density functional theory (DFT) computations, the catalytic performance of a series of single metal atoms supported on graphitic carbon nitride (g‐C3N4) for NRR is evaluated. Among all the candidates, the Gibbs free energy change of the potential‐determining step for five single‐atom catalysts (SACs), namely Ti, Co, Mo, W, and Pt atoms supported on g‐C3N4monolayer, is lower than that on the Ru(0001) stepped surface. In particular, the single tungsten (W) atom anchored on g‐C3N4(W@g‐C3N4) exhibits the highest catalytic activity toward NRR with a limiting potential of −0.35 V via associative enzymatic pathway, and can well suppress the competing hydrogen evolution reaction. The high NRR activity and selectivity of W@g‐C3N4are attributed to its inherent properties, such as significant positive charge and large spin moment on the W atom, excellent electrical conductivity, and moderate adsorption strength with NRR intermediates. This work opens up a new avenue of N2reduction for renewable energy supplies and helps guide future development of single‐atom catalysts for NRR and other related electrochemical process. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Save / Share this Record
  • Send to Email