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Plenary Session

Monday, June 13 • 17:30–19:00

f-Block Dinitrogen Chemistry: From Rarity to Catalysis in Three Ligand Modifications

Polly Arnold

Polly Arnold

University of California, Berkeley (USA)

Professor Polly L. Arnold received her MA degree in Chemistry from the University of Oxford and completed her D.Phil. under the supervision of Prof. F. Geoffrey N. Cloke at the University of Sussex. As a Fulbright Postdoctoral Fellow, Prof Arnold spent two years in Prof. Christopher C. Cummins’ laboratories at Massachusetts Institute of Technology. Immediately thereafter Prof. Arnold initiated her independent research program as a Lecturer in Chemistry at the University of Nottingham. In 2007, she moved to the University of Edinburgh as a Reader, and later, the Crum Brown Chair. Prof. Arnold is currently a Professor of Chemistry at the University of California, Berkeley and the Chemical Sciences Division Director of the Lawrence Berkeley National Laboratory.

Over the course of her career Prof. Arnold has published more than 150 papers and received numerous prestigious awards, including the Royal Society of Chemistry Sir Geoffrey Wilkinson Award for her work on transuranic organometallic chemistry. Prof. Arnold’s research focuses upon f-block homogeneous catalysis and fundamental actinide chemistry. In addition, she made the film “A Chemical Imbalance”, which is a call to action for simple changes to achieve equality of opportunity in science. In 2018 Prof. Arnold received an Order of the British Empire Award in the Queen’s birthday honours list for her contributions to chemistry and women in STEM.

Chemists have spent more than a century trying to make catalysts that can convert atmospheric dinitrogen to ammonia, or directly to amines under mild conditions. Hundreds of d-block complexes are now known to bind N2, and a few catalysts for N2 conversion to ammonia or tris(silyl)amine have been developed.

The binding of dinitrogen to any f-block metal cation was considered impossible until the turn of the millennium, but a small yet growing number of weakly-bound N2 complexes are now being reported. Studies of these weak binding interactions contribute to the fundamental understanding of bonding and electronic structure in these large, relativistic metals.

We will show what we have learnt about N2 binding to f-block centers over the last decade, and our recent development of the first molecular f-block complexes that can catalyse the reduction and functionalisation of dinitrogen. We will also discuss how structural control by the ligand framework can enable the first catalytic conversion of dinitrogen into a secondary silylamine by any metal.

 


Francis Lam,a Michael Trinh,a Anthony Wong,a Matthew Hernandez,a Rory Kelly,a Laurent Maron,b R. David Britt,c Polly L Arnold.a *

a. Dept. of Chemistry, University of California, Berkeley, and Lawrence Berkeley National Laboratory, Berkeley CA 94720, US.

b. Université de Toulouse and CNRS, INSA, UPS, CNRS, UMR 5215, LPCNO, F-31077 Toulouse, France. c. University of California, Davis, CA 95616, US.

References

  • Metallacyclic actinide catalysts for dinitrogen conversion to ammonia and secondary amines. P. L. Arnold, T. Ochiai, F. Y. T. Lam, R. P. Kelly, M. L. Seymour, L. Maron, Nature Chem. 2020, 12, 654-659. doi:10.1038/s41557-020-0457-9.
  • Dinuclear uranium complexation and manipulation using robust tetraaryloxides. J. A. L. Wells, M. L. Seymour, M. Suvova, P. L. Arnold, Dalton Trans. 2016, 45, 16026-16032. doi:10.1039/C6DT02630C.
  • Small molecule activation by uranium tris(aryloxides): Experimental and computational studies of binding of N2, coupling of CO, and deoxygenation insertion of CO2 under ambient conditions. S. M. Mansell, N. Kaltsoyannis, P. L. Arnold, Am. Chem. Soc. 2011, 133, 9036-9051. doi:10.1021/ja2019492.

 

Plenary Session

Tuesday, June 14 • 08:00–09:00

Facing Uncomfortable Truths and Driving Inclusive Excellence in Academic Scientific Research in Canada

Imogen Coe

Imogen Coe

Toronto Metropolitan University
(Canada)

Imogen R. Coe is a professor of chemistry and biology and former founding dean of the Faculty of Science at Toronto Metropolitan University in Toronto. She is also an affiliate scientist at St. Michael’s Hospital, Toronto, where her research group studies drug transporters. In addition to being an academic scientist, Dr. Coe is one of Canada’s leading advocates for organizational change towards inclusive excellence in research, particularly in science and medicine. She has advised academia, big tech, various research organizations & foundations as well as federal funding agencies on how to integrate equity, diversity and inclusion principles into research cultures across disciplines and at all levels. She is currently the Chair for EG1501 at NSERC, a scientific officer for Cell Biology – Physiology at CIHR and is completing a term as President of the Canadian Society of Molecular Biosciences. In addition to scientific contributions, she has published on inclusive leadership, misogyny in science and the need for intentional policy around EDI-infused organizational culture in diverse venues such as the Canadian Journal of Chemistry, the Lancet, iPolitics and the Globe and Mail. She is much in demand as a speaker and has received numerous awards for her advocacy work.

Research in the Canadian post-secondary sector exists within organizational cultures that reflect the structural and systemic racism, sexism, ableism and homophobia present in Canadian society. Academic research, like the rest of academia, continues to cling to the myth of meritocracy and this limits our ability to leverage all the talent available to us, to harness creativity and to drive innovation.  As academics and scientists need to get comfortable with the uncomfortable realities of that we, as human beings, are inherently biased and that we work within research cultures that are structurally inequitable. We need to learn how to mitigate inherent bias and re-calibrate our thinking and we need to challenge the status quo that protects power and privilege.  We need to be intentional about taking action to creating cultures of care that attract, retain, support and promote the widest breadth of research talent and ideas. Facing uncomfortable truths and taking action to re-calibrate our way of doing science can only lead to better and more rigorous science, more innovation, more creativity and ultimately better outcomes and outputs. This talk will discuss building the toolkit for change and suggest actions that individuals or institutions can take towards sustainable inclusive excellence in research in Canada. 

Plenary Session

Wednesday, June 15 • 08:00–09:00

Inventing Reactions for Green and Sustainable Chemical Syntheses

Chao-Jun Li

Chao-Jun Li

McGill University
(Canada, CIC Medal)

Dr. Chao-Jun Li received his Ph.D. at McGill University in 1992 and conducted research as an NSERC Postdoctoral Fellow at Stanford University from 1992-94. He then held a faculty position at Tulane University from 1994-2003. Since 2003, he has been a Canada Research Chair (Tier I) in Green Chemistry and an E. B. Eddy Chair at McGill University. He also served as the Co-Chair of the Canadian Green Chemistry/Engineering Network (2008-2016), Director of CFI Center for Green Chemistry/Green Chemicals, Director of NSERC CREATE for Green Chemistry, and Co-Director of FQRNT Center for Green Chemistry/Catalysis.

Dr. Li has received numerous prestigious awards worldwide including the US NSF CAREER Award (1997), US Presidential Green Chemistry Challenge Award (2001), Canadian Green Chemistry/Engineering Award (2010), Killam Research Fellow (2018), and Humboldt Research Award (2021). He has been elected a Fellow of the Royal Society of Canada (2012), the World Academy of Science (TWAS) (2016), European Academy of Sciences (2020), Royal Society of Chemistry (2007), AAAS (2012), CIC (2013), ACS (2015), and CCS (2020). His over 500 research articles on inventing new reactions for sustainable chemical synthesis have been cited widely (over 49,000 times, h-index=107). In 2007, the CSC listed Dr. Li’s work as among the 20 most important contributions to Canadian chemical research of the 20th century.

Website
Research Gate

The efficient making of new molecules is central to any chemical products in the pharmaceutical, agrochemical, fine chemical, material science and electronic industries.  On the other hand, the state-of-art chemical productions are generally based on non-renewable fossil-resources, often require lengthy transformations, and have low overall efficiency.  Towards future sustainability in chemical productions, innovations in chemical science and technologies are imperative, to transform readily available naturally abundant resources and functionality into high valued products directly, guided by the principles of Green Chemistry. C-C bond formation is the essence of chemical syntheses, among which organometallic reactions (nucleophilic addition, conjugate additions, and cross-couplings) play the central role.  For over 30 years, we have been exploring various novel C-C bond formation reactions that can simplify synthesis, decrease overall waste generation and maximize resource utilization, directly using naturally abundant feedstocks and functionalities.  In this talk, we will discuss our effort in this endeavor with a focus on more recent developments of this subject.

Plenary Session

Thursday, June 15 • 08:00–09:00

Shake, Rattle, & Roll: Capturing Snapshots of Radical Enzymes in Action

Cathy L. Drennan

Cathy L. Drennan

Howard Hughes Medical Institute

Cathy Drennan is a Professor and Investigator with the Howard Hughes Medical Institute and a Professor of Chemistry and Biology at the Massachusetts Institute of Technology. During her AB in chemistry from Vassar College she worked with Professor Miriam Rossi and discovered her passion for X-ray crystallography and for vitamin B12. But she did not head straight to graduate school, instead working as a high school teacher in West Branch, Iowa, for three years, teaching chemistry, biology, and physics by day and staging high school plays, such as The Importance of Being Earnest, by night. Realizing that teaching science and scientific research go hand in hand, Cathy enrolled in a PhD program at the University of Michigan to more fully experience the world of research. Carrying out her graduate studies in biological chemistry with the late Professor Martha L. Ludwig, Cathy used X-ray crystallography to show for the first time how vitamin B12 binds to a protein.

Following postdoctoral studies with Professor Douglas C. Rees at Caltech, Cathy joined the faculty of the Massachusetts Institute of Technology. Her laboratory seeks to understand how nature harnesses and re-directs the reactivity of enzyme metallocenters in order to perform challenging reactions. By combining X-ray crystallography and electron microscopy with other biophysical methods, the Drennan laboratory’s goal is to “visualize” molecular processes by obtaining snapshots of enzymes in action. Some of the proteins studied are newly characterized, and others have eluded structural characterization due to issues of oxygen sensitivity, conformational flexibility, protein heterogeneity, or structural complexity. The Drennan laboratory has specialized in tackling and solving these more challenging problems in structural biology. In total, Drennan is an author on over 175 publications, over 180 Protein Data Bank submissions, and has given over 200 invited talks. Her lab has provided several long-awaited structures, including the first structure of a class II ribonucleotide reductase (RNR), the first of a holocomplex of class I RNR (containing both subunits at 530 kDa), and the first structure of carbon monoxide dehydrogenase complexed with acetyl-CoA synthase at 310 kDa.

Cathy has been recognized with both teaching and research awards, including the Baker Award for Excellence in Undergraduate Teaching, the Edgerton Faculty Achievement Award, a Sloan Fellowship, an ASBMB-Schering-Plough Research Institute Scientific Achievement Award, a Presidential Early Career Award for Scientists and Engineers, a Searle Scholar Award, and the Dorothy Crowfoot Hodgkin Award from the Protein Society. She is an AAAS Fellow, an ASBMB Fellow, a MacVicar Faculty Fellow, and a member of the American Academy of Sciences. Cathy resides with her husband, Boston University Professor Sean J. Elliott, daughter Sammy, and labradoodle Casey in Newton, Massachusetts.

The use of radical-based chemistry allows for amazing transformations in living organisms. To carry out their functions, radical enzymes often need to be flexible and assume different conformational states, with units of the protein swinging back and forth to enable reactants to bind and products to leave while protecting radical-based intermediates. In this talk, the conformational gymnastics involved in ribonucleotide reduction are considered. Ribonucleotide reductases (RNRs) are radical enzymes that convert ribonucleotides (the building blocks of RNA) to deoxyribonucleotides (the building blocks of DNA). RNRs are targets for cancer chemotherapies and have been proposed to be candidates for antimicrobial therapies.  Here, I will describe how my lab has employed biophysical methods to interrogate how RNRs shake, rattle, and roll to accomplish their critical cellular function, including how RNR subunits come together to generate a 32-Å-long proton-coupled-electron-transport (PCET) pathway.

Plenary Session

Friday, June 17 • 08:00–09:00

Molecular Nanocarbons: From Precise Synthesis to Nanocarbon Biology

Kenichiro Itami

Kenichiro Itami

Nagoya University (Japan)

Professor Kenichiro Itami studied chemistry at Kyoto University, where he completed his doctoral studies with Prof. Yoshihiko Ito. He then took on an Assistant Professor position at the same university with Prof. Jun-ichi Yoshida. In 2005 he moved to Nagoya University as an Associate Professor with Prof. Ryoji Noyori, and was subsequently promoted to Full Professor in 2008. He has been the Director of the Institute of Transformative Bio-Molecules since 2012 and was the Research Director of the Itami Molecular Nanocarbon Project between 2013 and 2020. Professor Itami delivered more than 400 invited lectures and received numerous awards, including the Netherlands Scholar Award for Supramolecular Chemistry, the Chemical Society of Japan Award for Creative Work, the Nagase Prize, the Ta-Shue Chou Lectureship Award, the Arthur C. Cope Scholar Award, and the German Innovation Award.

The main emphasis of Prof. Itami’s research is on the development of synthetic methods, strategies, and concepts to solve challenging synthetic problems for generating as-yet unexplored molecules of significant interest. Representative projects include ideal chemical synthesis through C-H bond transformation, rapid synthesis of pharmaceutically relevant molecules and natural products, optoelectronic materials, as well as controlled bottom-up synthesis of structurally uniform nanocarbons such as carbon nanotubes, graphenes, and fullerenes.

Twitter: @Itamilab
Group website 

Our goal is the creation of super molecules, innovative functional molecules with significant properties and/or beautiful molecules. To this end, we have focused on catalyst-enabling synthetic chemistry with broad directions, including applications in molecular nanocarbons, pharmaceuticals, and plant/animal chemical biology, and the development of rapid molecule-assembly methods using unique catalysts. In particular, we have pioneered molecular nanocarbon science by the bottom-up synthesis of structurally uniform nanocarbons of fundamental and practical importance. Representative achievements include: (1) the development of single-step aromatic π-extension (APEX) methods for the rapid and programmable synthesis of nanocarbon molecules (Science 2018, Nature Commun. 2015, Nature Chem. 2015, Nature Commun. 2021); (2) the synthesis of carbon nanorings, nanobelts and pure nanotubes (ACIE 2009, Science 2017, Nature Chem. 2013, Nature Commun. 2018, Nature Commun. 2019, Nature Chem. 2021, Nature Synth. 2022); and (3) the synthesis of topologically unique nanocarbons such as warped nanographenes, carbon nanocages, all-benzene catenanes, trefoil knots, and infinitene (Science 2019, Nature Chem. 2013, Nature Catal. 2020, JACS 2022). In this talk, most recent beautiful molecular nanocarbons will be presented. We will also describe about our exciting new endevor trying to develop game-changing molecules for nanocarbon-based chemical biology.

Kenichiro Itami1,2,3

1 Institute of Transformative Bio-Molecules (WPI-ITbM), Nagoya University, Chikusa, Nagoya 464-8602, Japan

2 Department of Chemistry, Graduate School of Science, Nagoya University, Chikusa, Nagoya 464-8602, Japan

3 Institute of Chemistry, Academia Sinica, Nankang, Taipei 115, Taiwan