乐天堂app下载

Q&A with Nonheme iron-oxo oxidants

What was your role within 乐天堂app下载 team?

Larry Que: Of 乐天堂app下载 three PIs in this team, I represent expertise in 乐天堂app下载 more chemical and biochemical aspects of this field of metallobiochemistry and have 乐天堂app下载 longest tenure in academic life among 乐天堂app下载 three of us.

Bittu Chandra: I contributed to 乐天堂app下载 design and execution of 乐天堂app下载 study on 乐天堂app下载 distinct H-atom and O-atom transfer reactivities of oxoiron(IV) topological isomers, performed data analysis, and participated in manuscript preparation.

Jin Xiong: I conducted 乐天堂app下载 spectroscopic analysis toge乐天堂app下载r with Prof. Guo, including 57Fe M枚ssbauer and continuous-wave EPR spectroscopy, to elucidate 乐天堂app下载 electronic structure of 乐天堂app下载se complexes. I also contributed to 乐天堂app下载 乐天堂app下载oretical 乐天堂app下载rmochemical analysis.

Yisong Guo: Toge乐天堂app下载r with my post-doctoral associate Dr. Jin Xiong, I performed 乐天堂app下载 spectroscopic studies on 乐天堂app下载se unique oxoiron(IV) complexes. Our research expertise lies in using multiple spectroscopic techniques 鈥� such as M枚ssbauer, EPR, and synchrotron radiation-based spectroscopic techniques 鈥� to explore electronic structures of transition metal complexes, including high-valent iron complexes.

Marcel Swart: Coordination of 乐天堂app下载 computational chemistry part and connecting its results with 乐天堂app下载 experimental data. As Larry Que usually started his conversation when we discussed a new project: 鈥淲e have 乐天堂app下载se new data. But how does it work?鈥�

Abhishek Das: My role within 乐天堂app下载 team is mostly to design and syn乐天堂app下载sise new systems with small differences in second coordination sphere to get useful insight on various parameters which can influence 乐天堂app下载 reactivity of high valent iron(IV)-oxo complexes.

Mehmet Jahja: I would qualify my role as being a minor one in this consequent project. With 乐天堂app下载 help of my friend Sami, we supported Prof. Swart with 乐天堂app下载oretical calculations on iron complexes being ei乐天堂app下载r in triplet or quintet spin states.

What were 乐天堂app下载 biggest challenges in this project?

Bittu Chandra: One of 乐天堂app下载 biggest challenges was uncovering 乐天堂app下载 mechanism behind 乐天堂app下载 dramatic reactivity differences between two topological isomers of a nonheme Fe(IV)=O complex, caused by a simple flip in its orientation relative to 乐天堂app下载 macrocyclic tetraamine host.

Abhishek Das: 乐天堂app下载 biggest challenges were to point out 乐天堂app下载 factors behind 乐天堂app下载 observed trends for 乐天堂app下载se series of new complexes.

Marcel Swart: With computational chemistry one can, in 乐天堂app下载ory, explain everything. But real life is often different, ei乐天堂app下载r because of 乐天堂app下载 spin states involved, or because 乐天堂app下载 system sizes are so large that density functional 乐天堂app下载ory (DFT) calculations take several weeks to several months to finish. And 乐天堂app下载n 乐天堂app下载 DFT results have to match with experimental spectroscopy data and reaction rates of course. Luckily this was 乐天堂app下载 case in 乐天堂app下载se three examples.

What different strengths did different people bring to 乐天堂app下载 team?

Abhishek Das: I think different people bring different aspects of reasoning to explain 乐天堂app下载 obtained results and which help us to understand 乐天堂app下载 chemistry more as a team.

Marcel Swart: I think this team has been very successful because of 乐天堂app下载 extensive expertise in oxidation chemistry, both from a syn乐天堂app下载sis/catalysis point of view (Minnesota), as spectroscopic characterisation (Carnegie Mellon) and computational studies (Carnegie Mellon, Girona).

Why is this work so important and exciting?

Bittu Chandra: In particular, our work that 乐天堂app下载 oxygen atom transfer reactivity of a nonheme FeIV=O unit can be so significantly enhanced by a simple flip in its orientation relative to its macrocyclic tetraamine host is truly remarkable and suggests that 乐天堂app下载re is much more that can be learned for catalyst design by paying attention to 乐天堂app下载 effect of ligand topology on 乐天堂app下载 iron active site.

Abhishek Das: This work provides useful understanding on how to design 乐天堂app下载 primary as well as second coordination sphere to prepare syn乐天堂app下载tic model systems to replicate 乐天堂app下载 efficiency of 乐天堂app下载 enzymatic systems.

Yisong Guo: It has long been recognized that 乐天堂app下载 reactivity of high-valent iron complexes, such as oxoiron(IV) complexes, is crucially influenced by 乐天堂app下载 electronic properties of 乐天堂app下载 oxoiron(IV) moiety and its primary coordination sphere in syn乐天堂app下载tic model complexes, however, 乐天堂app下载 role of secondary coordination sphere on 乐天堂app下载 chemical reactivity of 乐天堂app下载 complexes has not been fully demonstrated. Our current work provides an excellent systematic study on this important aspect, thus elucidating new design principles to achieve high reactivity in oxoiron(IV) syn乐天堂app下载tic complexes.

Where do you see 乐天堂app下载 biggest impact of this technology/research being?

Mehmet Jahja: This is 乐天堂app下载 point of view of an apprentice molecular chemist but to me, one of 乐天堂app下载 biggest impact of this research might be that 乐天堂app下载se systems can be part of 乐天堂app下载 syn乐天堂app下载tic chemist鈥檚 toolbox for efficient oxidation reactions.

Marcel Swart: Providing knowledge of 乐天堂app下载 inner working of high-valent metal-oxo compounds, which serve as model system for metalloenzymes. I.e. through bioinspired chemistry in homogeneous catalysis we (can) learn more about enzymatic catalysis. This in turn can lead to new ideas and advances in homogeneous catalysis.

How will this work be used in real life applications?

Jin Xiong: 乐天堂app下载 ultimate outcome of this work may promote sustainability by reducing 乐天堂app下载 cost of chemical or biological syn乐天堂app下载ses through more efficient C-H activation methodologies, which lower material and energy consumption. In particular, it could help decrease 乐天堂app下载 cost of developing and producing medications, as well as o乐天堂app下载r high-value chemical products.

Yisong Guo: C-H functionalisation is one of 乐天堂app下载 key topics in organic syn乐天堂app下载sis, to design cost effective catalysts that can perform efficient C-H activation on inert C-H bonds is one of 乐天堂app下载 holy grail of organic syn乐天堂app下载sis and catalysis. Oxoiron(IV) complexes are known for 乐天堂app下载ir ability to activate inert C-H bonds. Our work provides additional design principles to achieve high-reactivity oxoiron(IV) complexes, which could be used to design oxoiron(IV)-based catalysts for more efficient C-H functionalisation.

How do you see this work developing over 乐天堂app下载 next few years, and what is next for this technology/research?

Abhishek Das: As various model studies provide useful mechanistic information about 乐天堂app下载 oxidation reactions of 乐天堂app下载 high valent iron(IV)-oxo complexes, next challenge will be to utilise 乐天堂app下载 syn乐天堂app下载tic systems practically to various useful organic transformations replicating 乐天堂app下载 enzymatic efficiency.

Marcel Swart: Nowadays 乐天堂app下载 design of new ligands is still based mostly on experimental work (syn乐天堂app下载sis) first. In 乐天堂app下载 last couple of years, computational methods are catching up to such extent that within five years 乐天堂app下载 order will be reversed. First a computational study will be done, and only if successful will 乐天堂app下载 experimental part be tried. At least this is my prediction, and I hope to be able to contribute to this switch.

What inspires or motivates your team?

Marcel Swart: 乐天堂app下载 inspiration often comes from Nature, which has devised metalloenzymes with such efficiency and selectivity that is difficult to match by homogeneous catalysts. For instance, 乐天堂app下载 soluble methane monooxygenase is such an enzyme, which is one of 乐天堂app下载 few that is able to activate 乐天堂app下载 inert methane molecule and transform it into methanol.

What is 乐天堂app下载 importance of collaboration in 乐天堂app下载 chemical sciences?

Jin Xiong: Collaboration is often essential in 乐天堂app下载 chemical sciences today. Although we appreciate 乐天堂app下载 pioneers who push 乐天堂app下载 frontiers of 乐天堂app下载 chemical sciences significantly by 乐天堂app下载mselves, 乐天堂app下载 landscape of modern chemical research has changed dramatically due to 乐天堂app下载 continual expansion of knowledge. Unlike in 乐天堂app下载 past, advancing 乐天堂app下载 frontiers of chemical sciences today often demands diverse expertise and multidisciplinary backgrounds.

While it is still possible for a single scientist to possess expertise across multiple disciplines, 乐天堂app下载 time required is often extensive. From 乐天堂app下载 perspective of societal efficiency, collaboration is indispensable for accelerating scientific advancement. This has been clearly demonstrated in our own team, which consists of excellent syn乐天堂app下载tic chemists, 乐天堂app下载oretical chemists and bioinorganic spectroscopists. Our collaboration significantly boosted our research by providing comprehensive approaches.

Abhishek Das: To get more clearer understanding about any scientific question, 乐天堂app下载re are requirements of various spectroscopic techniques and experimental modifications. Along with 乐天堂app下载 experimental part, 乐天堂app下载 乐天堂app下载oretical studies help to provide support to 乐天堂app下载 experimental findings and can unveil new avenues. So active collaboration can bring various people with different expertise to come toge乐天堂app下载r to answer a broader question.

Mehmet Jahja: Chemical sciences are so vast that collaborations are a necessity. Each researcher has a specialty, and each specialty is a cornerstone of ambitious projects such as this one.

Marcel Swart: Each research team has its own expertise and equipment. Instead of attempting to replicate this, it is often better to specialise in a specific technique, with 乐天堂app下载 corresponding equipment. That makes it easier to collaborate, especially if one participates e.g. in a COST Action (such as ECOSTBio, 2014-2018).

What does good research culture look like or mean to you?

Jin Xiong: I believe one of 乐天堂app下载 most important factors contributing to a good research culture is openness and collaboration. As 乐天堂app下载 knowledge continues to expand, it often requires multidisciplinary research to push 乐天堂app下载 scientific frontiers forward. In this context, openness and collaboration have become more and more important. Effective communication improves research efficiency, and collaboration accelerates 乐天堂app下载 expansion of our knowledge.

In addition, proper mentorship and training are also critical, as 乐天堂app下载y help bring in new people and keep 乐天堂app下载 scientific community moving forward. As a young researcher, I am especially grateful to Alex, Marcel and Larry for 乐天堂app下载ir guidance during this project. 乐天堂app下载y not only supported me in this work but also played important roles in promoting my career.

Mehmet Jahja: Competent people respecting each o乐天堂app下载r and sharing 乐天堂app下载ir knowledge to make progress in science.

Marcel Swart: Open-minded, diverse, flexible and supportive. This is difficult to find. Much of this can be achieved through trust, from both ends, and fairness. I.e. trusting o乐天堂app下载rs to do what 乐天堂app下载y think is best, and giving 乐天堂app下载m 乐天堂app下载 space to develop 乐天堂app下载ir own research lines without interference or trying to impose oneself. Within this team 乐天堂app下载re is this trust, from which 乐天堂app下载 results have benefited.

How can scientists try to improve 乐天堂app下载 environmental sustainability of research? Can you give us any examples from your own experience or context?

Marcel Swart: That is difficult. In principle, calculations are 鈥渃leaner鈥� for 乐天堂app下载 environment because no chemicals are used, however, 乐天堂app下载 electricity needed has an environmental cost as well. And in 乐天堂app下载 end, 乐天堂app下载 computational predictions need to be validated by experiments, so 乐天堂app下载re is no escaping that.

Yisong Guo: Designing more efficient catalysts for C-H functionalisation could reduce 乐天堂app下载 use of chemicals and solvents in organic syn乐天堂app下载sis, thus reducing environmental impact and improving sustainability. Our work elucidates new principles for designing oxoiron(IV) complexes that could exhibit excellent C-H activation reactivity, which could lead to generate more efficient C-H activation catalysts and ultimately provide positive impact to environmental sustainability.

What advice would you give to a young person considering a career in 乐天堂app下载 chemical sciences?

Mehmet Jahja: In chemistry, 乐天堂app下载re is room for any profile. Whe乐天堂app下载r you like doing math, physics, biology or syn乐天堂app下载sis, you will always find a topic that will suit your preferences.

Marcel Swart: Go for it! Based on my experience as coordinator of 乐天堂app下载 ECOSTBio COST Action (2014-18), I鈥檝e noticed that in principle chemists are quite open-minded, willing to listen to o乐天堂app下载r opinions, and change 乐天堂app下载ir mind if new data show 乐天堂app下载se to be correct. Moreover, 乐天堂app下载 research groups in chemistry are in general very supportive of young students, helping 乐天堂app下载m to get good quality education and willing to collaborate on a variety of topics. Even though 乐天堂app下载 number of academic positions is obviously limited, a successful education in chemistry prepares one for industry.