Nicholas C. Nelson's research while affiliated with Pacific Northwest National Laboratory and other places
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Publications (5)
Dilution of Pd/TiO2 with neat TiO2 results in the formation of atomically dispersed Pd under reverse water–gas shift (rWGS) reaction conditions at 400 °C and a several‐fold increase in activity.
Abstract
The application of single‐atom catalysts (SACs) to high‐temperature hydrogenation requires materials that thermodynamically favor metal atom isol...
Expanding the application scope of single‐atom catalysts (SACs) to high‐temperature hydrogenation requires materials that thermodynamically favor metal atom isolation over cluster formation under these conditions. Here, we show that Pd can be predominantly dispersed as isolated atoms onto TiO 2 during the reverse water‐gas shift (rWGS) reaction at...
Identifying the role of oxide supports in transition metal catalysis is critical toward our understanding of heterogeneous catalysis. The water-gas shift (WGS) reaction is a prototypical example where oxide support dictates catalytic activity, yet the cause for this remains uncertain. Herein, we show that a single descriptor—the equilibrium constan...
Identifying the role of oxide supports in transition metal catalysis is critical toward our understanding of heterogeneous catalysis. The water-gas shift (WGS) reaction is a prototypical example where oxide support dictates catalytic activity, yet the cause for this remains uncertain. Herein, we show that a single descriptor—the equilibrium constan...
Definitive experimental proof for catalytic pathways and active sites during the low-temperature water-gas shift reaction remains elusive. Herein, we combine spectroscopic, kinetic and computational analyses to address the decades-long mechanistic controversy by studying the reverse water-gas shift over Pd/Al2O3. Isotopic transient kinetic analysis...
Citations
... 31 Additionally, the first report, in 1991, on single atom detection by EELS was also about uranium atoms on carbon. 32 In 2015, the visualization of reacting PtSA deposited on carbon support in chemical reactions was reported. 33 All these progresses in surface science and modelling allow today an easier characterization of SA on carbon materials. ...
... However, nickel-based catalysts were also susceptible to be deactivated by CH 4 decomposition or coke formation via CO disproportionation (Bourdouard reaction), as well as by sulfur poisoning. Noble metals, such as Ru [12,22,23], Pd [24][25][26][27], Pt [6,28] and Rh [29][30][31], can also consist of catalysts and be active for methanation. And Ru exhibits the highest catalytic activity over a wide range of temperatures among them [32]. ...
... Previous work by Sharafi et al. using Raman and X-ray photo-emission spectroscopy (XPS) revealed the existence of thick layers (∼5-10 nm) of Li 2 CO 3 on the Li 7 La 3 Zr 2 O 12 surfaces, upon exposure to air. 21,23 The same authors also detected LiOH on the Li 7 makes it potentially relevant for the water-gas shift reaction, 44,45 while the strong chemisorption of CO 2 makes Li 7 La 3 Zr 2 O 12 a promising dual functional material for CO 2 capture and conversion. 46,47 Hence, in the context of catalysis, Li 7 La 3 Zr 2 O 12 appears an excellent catalyst support to investigate reactions of CO 2 activation and water splitting, respectively. ...
... This suggested that the desorption of CO 2 was promoted in the photo-driven regime, thus preventing bicarbonate formation. [18] No other new peaks were observed, indicating that the hot electrons created by Cu nanoparticles in the plasmonic LD-Cu catalysts did not change the main reaction path or produce any new intermediates, but simply promoted the original carboxyl reaction mechanism by overcoming the high barriers of water activation and dissociation. Figure S17 shows the integrated peak intensities for the different groups (*H 2 O, *COO À and *CO 2 ) with time during the in situ DRIFTS experiment under dark and light conditions. ...
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