Editorial pubs.acs.org/acscatalysis
The Community Comments on the Most Important ACS Catalysis Papers Published in 2012−2013
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unfunctionalized trisubstituted and tetrasubstituted alkenes. The origin of electronic influences, the role of redox activity, and elucidation of mechanistic pathways were all investigated. These results provide important insight and hints for new ligand and catalyst designs. This work inspired me in the search for new hydrogenation catalysts and strategies for catalyst design in asymmetric hydrogenation.” Other papers published in 2012 were also cited with thoughtful descriptions of how they impacted a reader’s thinking about catalysis. For example, the paper by Nørskov and co-workers, “Universality in Oxygen Reduction Electrocatalysis on Metal Surfaces” (DOI: 10.1021/cs300227s),4 was noted for its impact on continuing work rationalizing the oxygen reduction reaction. A reader remarked “the oxygen reduction is a reaction of fundamental scientific and technological importance, representing an important bottleneck for fuel cells, while in biology, the oxygen reduction reaction is carried out by cytochrome c oxidase and is fundamental to life. In this paper, the authors identify a fundamental limit for the efficiency of any metal catalyst for aqueous oxygen reduction on metal surfaces. This shows that no metal catalyst could have an overpotential lower than η = 0.37 ± 0.1 V. Further, this collapses nearly 30 years of experimental data into a single plot and provides a structure−activity descriptor. The structure− activity descriptor has subsequently been used for new catalyst discovery already.5 Building on this, similar fundamental limits have been extended by others to non-aqueous oxygen reduction on metal surfaces.”6 In another example, the work by Medlin, van Bokhoven, and co-workers (DOI: 10.1021/ cs300378p)7 offered an example of “the rational design of a modified catalyst system offering the ability to switch selectivity in a chemoselective reaction, offering high selectivity and conversion to the desired product. The ideas in this paper are clearly transferable to other catalytic systems.” Several papers from 2013 were also highlighted. In the area of hydrogen production and storage, the design of ligands that facilitate proton shuttling has become an important strategy for efficient and active catalysts. One example was the work of Wang, Muckerman, Fujita, and Himeda (DOI: 10.1021/ cs400172j),8 where a reader remarked “this paper showed that the half-sandwich Cp*Ir complex coordinated by orthoOH-functionalized bipyridine (namely, a proton-response ligand) showed ultrahigh catalytic CO2 hydrogenation ability. The ortho-OH reversibly generates an ortho-oxyanion, which profoundly affects reactivity and offers good performance in water. Building on this, others have used similar Cp*Ir complexes in the hydrogenation of biobased chemicals, such as 5-HMF.9,10 I believe the “proton-response” strategy will be fruitfully explored by the catalysis community as a basis for catalyst design.”
very Fall, the chemical community informally discusses the state of their field around the time that Nobel Prizes are announced. It is a natural time to reflect and consider the major discoveries that led to evolving trends in the discipline, and to hypothesize about what the future will hold for each subdiscipline in catalysis. Recently, I attended the 24th Solvay Conference on Chemistry: Catalysis in Chemistry and Biology, in Brussels. The presentations and discussions spanned the full breadth of catalysis, including discussions on molecular catalysis, heterogeneous catalysis, and biocatalysis/enzymology. Seasoned Nobel Laureates (Marcus, Wüthricht, Grubbs, Ertl), U.S. National Medal of Science winners (Stubbe, Klinman), as well as new Nobel winners (Feringa) with expertise in catalysis all contributed their thoughts on the future of the field. The assembled researchers sought to find commonalities between the various subdisciplines of catalysis, discussing unifying themes. It is refreshing to see the fields moving closer together, a trend represented by the launch of ACS Catalysis in 2010. In this year’s June issue of ACS Catalysis, I asked the community to consider a few questions about papers that appeared in the journal.1 Specifically, I asked:
• Which original research papers published in ACS Catalysis in 2012 or 2013 have affected your thinking about catalysis in a significant way? • What papers from this period in the journal will authors still be reading and citing in 2022, that is, 10 years later? Below, I share with you some of the responses we received. Two papers shared the most recommendations, both published in 2012. The first was “Production of 5Hydroxymethylfurfural from Glucose Using a Combination of Lewis and Brønsted Acid Catalysts in Water in a Biphasic Reactor with an Alkylphenol Solvent,” by Shanks, Dumesic, and co-workers (DOI: 10.1021/cs300192z).2 With the nominations came comments such as “this was an early demonstration of a cascade process for biomass conversion utilizing a renewable solvent for efficient separation of 5-HMF; this approach is being adapted by many other groups for the synthesis of this valuable platform chemical.” The second paper that shared the same number of nominations was “High-Activity Iron Catalysts for the Hydrogenation of Hindered, Unfunctionalized Alkenes,” by Chirik and co-workers (DOI: 10.1021/cs300358m).3 A member of the community commented: “this work is on the design of highly active iron catalysts and their application in the hydrogenation of hindered, unfunctionalized alkenes, which is one of the most challenging substrate classes for homogeneous hydrogenation catalysts. Precious metal compounds have dominated the catalyst landscape in hydrogenation. Iron is a good choice for displacement of precious metals due to its low toxicity and high abundance. However, examples of iron catalysts that operate under mild conditions with high activity and a broad substrate scope are rare. In this paper, the authors demonstrated that more electron-rich iron dinitrogen pincer complexes are effective for the catalytic hydrogenation of © 2016 American Chemical Society
Published: November 4, 2016 7977
DOI: 10.1021/acscatal.6b03042 ACS Catal. 2016, 6, 7977−7978
ACS Catalysis
Editorial
I conclude by sharing a few interesting observations about the responses received from the readership. In reviewing the array of papers identified by the community, which numbered about 50, there was no obvious correlation with the papers identified and the number of times the papers were cited in the scientific literature. The number of citations to the nominated papers ranged from as low as 7 to as high as 200. Additionally, there was great diversity in the papers cited and diversity in the location, experience, and affiliation of the respondents. The catalysis community is truly a global one. I want to thank everyone who responded to this inquiry. It was interesting to read all the responses. While the above excerpts only represent a fraction of those received, the comments are representative of the overall submissions.11 From my perspective as Editor-in-Chief, it is wonderful to be a part of such an energetic and vibrant community.
Christopher W. Jones, Editor-in-Chief
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Georgia Institute of Technology
AUTHOR INFORMATION
Notes
Views expressed in this editorial are those of the author and not necessarily the views of the ACS.
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REFERENCES
(1) Jones, C. W. ACS Catal. 2016, 6, 4046. (2) Pagán-Torres, Y. J.; Wang, T.; Gallo, J. M. R.; Shanks, B. H.; Dumesic, J. A. ACS Catal. 2012, 2, 930−934. (3) Yu, R. P.; Darmon, J. M.; Hoyt, J. M.; Margulieux, G. W.; Turner, Z. R.; Chirik, P. J. ACS Catal. 2012, 2, 1760−1764. (4) Viswanathan, V.; Hansen, H. A.; Rossmeisl, J.; Nørskov, J. K. ACS Catal. 2012, 2, 1654−1660. (5) Holewinski, A.; Idrobo, J.-C.; Linic, S. Nat. Chem. 2014, 6, 828− 834. (6) Krishnamurthy, D.; Hansen, H. A.; Viswanathan, V. ACS Energy Lett. 2016, 1, 162−168. (7) Makosch, M.; Lin, W.-I.; Bumbálek, V.; Sá, J.; Medlin, J. W.; Hungerbühler, K.; van Bokhoven, J. A. ACS Catal. 2012, 2, 2079− 2081. (8) Wang, W.-H.; Muckerman, J. T.; Fujita, E.; Himeda, Y. ACS Catal. 2013, 3, 856−860. (9) Xu, Z.; Yan, P.; Xu, W.; Liu, X.; Xia, Z.; Chung, B.; Jia, S.; Zhang, Z. C. ACS Catal. 2015, 5, 788−792. (10) Xu, Z.; Yan, P.; Li, H.; Liu, K.; Liu, X.; Jia, S.; Zhang, Z. C. ACS Catal. 2016, 6, 3784−3788. (11) Note that responses quoted above are excerpts of longer responses received in many cases. In some cases, the text was modified slightly for flow, though the tone and tenor of the comments were maintained in all cases.
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DOI: 10.1021/acscatal.6b03042 ACS Catal. 2016, 6, 7977−7978
