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.


Title: High-area alumina supported Cu–Ce atomic species for water–gas shift reaction
Atomically dispersed cerium species, anchored to high-area alumina by unsaturated penta-coordinated aluminum, strongly interact with atomically dispersed Cu species to provide active centers for water–gas shift reaction (WGSR).  more » « less
Award ID(s):
2247571
PAR ID:
10595868
Author(s) / Creator(s):
; ; ;
Publisher / Repository:
The Royal Society of Chemistry (RSC)
Date Published:
Journal Name:
Chemical Communications
Volume:
60
Issue:
68
ISSN:
1359-7345
Page Range / eLocation ID:
9093 to 9096
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Atomically dispersed catalysts have been shown highly active for preferential oxidation of carbon monoxide in the presence of excess hydrogen (PROX). However, their stability has been less than ideal. We show here that the introduction of a structural component to minimize diffusion of the active metal center can greatly improve the stability without compromising the activity. Using an Ir dinuclear heterogeneous catalyst (DHC) as a study platform, we identify two types of oxygen species, interfacial and bridge, that work in concert to enable both activity and stability. The work sheds important light on the synergistic effect between the active metal center and the supporting substrate and may find broad applications for the use of atomically dispersed catalysts. 
    more » « less
  2. Abstract Atomically dispersed and nitrogen coordinated single metal sites (M‐N‐C, M=Fe, Co, Ni, Mn) are the popular platinum group‐metal (PGM)‐free catalysts for many electrochemical reactions. Traditional wet‐chemistry catalyst synthesis often requires complex procedures with unsatisfied reproducibility and scalability. Here, we report a facile chemical vapor deposition (CVD) strategy to synthesize the promising M‐N‐C catalysts. The deposition of gaseous 2‐methylimidazole onto M‐doped ZnO substrates, followed by an in situ thermal activation, effectively generated single metal sites well dispersed into porous carbon. In particular, an optimal CVD‐derived Fe‐N‐C catalyst exclusively contains atomically dispersed FeN4sites with increased Fe loading relative to other catalysts from wet‐chemistry synthesis. The catalyst exhibited outstanding oxygen‐reduction activity in acidic electrolytes, which was further studied in proton‐exchange membrane fuel cells with encouraging performance. 
    more » « less
  3. Abstract Atmospheric NO2is of great concern due to its adverse effects on human health and the environment, motivating research on NO2detection and remediation. Existing low-cost room-temperature NO2sensors often suffer from low sensitivity at the ppb level or long recovery times, reflecting the trade-off between sensor response and recovery time. Here, we report an atomically dispersed metal ion strategy to address it. We discover that bimetallic PbCdSe quantum dot (QD) gels containing atomically dispersed Pb ionic sites achieve the optimal combination of strong sensor response and fast recovery, leading to a high-performance room-temperature p-type semiconductor NO2sensor as characterized by a combination of ultra–low limit of detection, high sensitivity and stability, fast response and recovery. With the help of theoretical calculations, we reveal the high performance of the PbCdSe QD gel arises from the unique tuning effects of Pb ionic sites on NO2binding at their neighboring Cd sites. 
    more » « less
  4. Abstract Developing eco‐friendly electrochemical devices for electrosynthesis, fuel cells (FCs), and metal‐air batteries (MABs) requires precisely designing the electronic pathway in the oxygen reduction reaction (ORR) process. Understanding the principle of developing low‐cost, highly active, and stable catalysts helps to reduce the usage of noble metals in ORR. Atomically dispersed metal catalysts (ADMCs) emerge as promising alternatives to replace commercial noble metals due to their high utilization of active metal atoms, high intrinsic activity, and controllable coordination environments. In this review, the research tendency and reaction mechanisms in ORR are first summarized. The basic principles concerning the geometric size and chemical coordination of two‐electron ORR (2eORR) catalysts were then discussed, aiming to outline the evolution of material design from 2eORR to four‐electron ORR (4eORR). Subsequently, recent advances in ADMCs primarily investigated for the 4eORR are well‐documented. These advances encompass studies on M−N−C coordination, light heteroatom doping, dual‐metal atoms‐based coordination, and interaction between nanoparticle (NPs)/nanoclusters (NCs) and atomically dispersed metals (ADMs). Finally, the setups for 2/4eORR applications, key challenges, and opportunities in the future design of ADMCs for the ORR are highlighted. 
    more » « less
  5. Abstract Oxide supports with well‐defined shapes enable investigations on the effects of surface structure on metal–support interactions and correlations to catalytic activity and selectivity. Here, a modified atomic layer deposition technique was developed to achieve ultra‐low loadings (8–16 ppm) of Pt on shaped ceria nanocrystals. Using octahedra and cubes, which expose exclusively (111) and (100) surfaces, respectively, the effect of CeO2surface facet on Pt‐CeO2interactions under reducing conditions was revealed. Strong electronic interactions result in electron‐deficient Pt species on CeO2(111) after reduction, which increased the stability of the atomically dispersed Pt. This afforded significantly higher NMR signal enhancement in parahydrogen‐induced polarization experiments compared with the electron‐rich platinum on CeO2(100), and a factor of two higher pairwise selectivity (6.1 %) in the hydrogenation of propene than any previously reported monometallic heterogeneous Pt catalyst. 
    more » « less