{Despite|Regardless of|In spite of} decades of {effort|work}, no earth abundant homogeneous catalysts {have been|happen to be|have already been} {discovered|found} {that can|that may|that will|that could|which will|which can} selectively oxidize methane to methanol. We exploit active {learning|studying|understanding|finding out|mastering} to simultaneously optimize methane activation and methanol release calculated with machine {learning|studying|understanding|finding out|mastering} (ML)-accelerated density functional theory (DFT) {in a|inside a|within a} space of 16M candidate catalysts with novel macrocycles. By constructing these macrocycles from fragments inspired by synthesized compounds, we {ensure|make sure|make certain|guarantee|assure} synthetic realism in our computational search. Our large-scale search reveals that low spin Fe(II) compounds paired with {strong|powerful|robust|sturdy} field (e.g. P or S-coordinating) ligands {have the|possess the} {best|very best|greatest|ideal|finest|most effective} energetic tradeoff {between|in between|among|amongst|involving} hydrogen atom transfer (HAT) and methanol release. This observation is distinct from prior efforts {that have|which have} focused on {high|higher} spin Fe(II) with weak field ligands. By decoupling equatorial and axial ligand effects, we {determine|figure out|decide|establish|ascertain|identify} that negatively charged axial ligands are {critical|crucial|vital|essential|important} for {more|much more|a lot more|far more|additional|extra} {rapid|fast|speedy} release of methanol and, {higher|greater|larger} valency metals (i.e., M(III) vs M(II)) are unlikely {to be|to become} {suitable|appropriate} for methanol release. With {full|complete} characterization of barrier heights, we confirmed that optimizing for HAT {did not|didn’t} {lead to|result in|bring about|cause} {large|big|huge|massive|substantial|significant} oxo formation barriers. Energetic span {analysis|evaluation} revealed {designs|styles} for an intermediate spin Mn(II) catalyst {and a|along with a|as well as a|plus a|and also a|in addition to a} low spin Fe(II) catalyst that would {lead to|result in|bring about|cause} {good|great|excellent|very good|fantastic|superior} turnover frequencies. This active {learning|studying|understanding|finding out|mastering} {approach|method|strategy} is {expected|anticipated} {to be|to become} {beneficial|advantageous|helpful|useful|valuable|effective} for search of {large|big|huge|massive|substantial|significant} catalyst spaces {where|exactly where} no prior {designs|styles} {have been|happen to be|have already been} identified and {where|exactly where} linear scaling relationships {between|in between|among|amongst|involving} reaction energies or barriers {may|might|could|may possibly|may well|may perhaps} be {limited|restricted} or unknown. 2-Amino-5-methoxyphenol custom synthesis Bis(cyclooctadiene)dichlorodirhodium Chemical name PMID:32472497
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