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000481804 0247_ $$2doi$$a10.26434/chemrxiv-2022-jvtgw
000481804 0247_ $$2datacite_doi$$a10.3204/PUBDB-2022-04572
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000481804 037__ $$aPUBDB-2022-04572
000481804 041__ $$aEnglish
000481804 1001_ $$0P:(DE-H253)PIP1092788$$aCaserta, Giorgio$$b0$$eCorresponding author
000481804 245__ $$aActive site assembly of [NiFe]-hydrogenase scrutinized on the basis of purified maturation intermediates
000481804 260__ $$c2022
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000481804 500__ $$aFunding:Einstein Foundation Berlin: grant number EVF-2016-277;SPP 1927 “Iron Sulfur for Life”: grants: DE1877/1-1 and 311062227;Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515
000481804 520__ $$a[NiFe]-hydrogenases are biotechnologically relevant enzymes catalyzing the reversible splitting of H$_2$ into 2 e$^- $ and 2 H$^+$ under ambient conditions. Catalysis takes place at the heterobimetallic NiFe(CN)$_2$(CO) center, whose multistep biosynthesis involves careful handling of two transition metals as well as potentially harmful CO and CN$^–$ molecules. Herein, we investigated the sequential assembly of the [NiFe]-cofactor, previously based on primarily indirect evidence, using four different purified maturation intermediates of the catalytic subunit, HoxG, of the O$_2$-tolerant membrane-bound hydrogenase from Cupriavidus necator. These included the cofactor-free apo-HoxG, a nickel-free version carrying only the Fe(CN)$_2$(CO) fragment, a precursor that contained all cofactor components but remained redox-inactive, and the fully mature HoxG. Through biochemical analyses combined with comprehensive spectroscopic investigation using infrared, electronic paramagnetic resonance, Mössbauer, X-ray absorption, and nuclear resonance vibrational spectroscopies, we obtained detailed insight into the sophisticated maturation process of [NiFe]-hydrogenase.
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000481804 7001_ $$0P:(DE-HGF)0$$aHartmann, Sven$$b1
000481804 7001_ $$0P:(DE-H253)PIP1085616$$avan Stappen, Casey$$b2
000481804 7001_ $$0P:(DE-HGF)0$$aKarafoulidi Retsou, Chara$$b3
000481804 7001_ $$0P:(DE-H253)PIP1100547$$aLorent, Christian$$b4
000481804 7001_ $$0P:(DE-HGF)0$$aYelin, Stefan$$b5
000481804 7001_ $$0P:(DE-HGF)0$$aKeck, Matthias$$b6
000481804 7001_ $$0P:(DE-HGF)0$$aSchoknecht, Janna$$b7
000481804 7001_ $$0P:(DE-H253)PIP1016663$$aSergueev, Ilya$$b8
000481804 7001_ $$0P:(DE-HGF)0$$aYoda, Yoshitaka$$b9
000481804 7001_ $$0P:(DE-HGF)0$$aHildebrandt, Peter$$b10
000481804 7001_ $$0P:(DE-HGF)0$$aLimberg, Christian$$b11
000481804 7001_ $$0P:(DE-H253)PIP1015325$$aDeBeer, Serena$$b12
000481804 7001_ $$0P:(DE-H253)PIP1100480$$aZebger, Ingo$$b13
000481804 7001_ $$0P:(DE-HGF)0$$aFrielingsdorf, Stefan$$b14$$eCorresponding author
000481804 7001_ $$0P:(DE-HGF)0$$aLenz, Oliver$$b15$$eCorresponding author
000481804 773__ $$a10.26434/chemrxiv-2022-jvtgw
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000481804 9101_ $$0I:(DE-HGF)0$$6P:(DE-HGF)0$$aTechnische Universität Berlin$$b1
000481804 9101_ $$0I:(DE-HGF)0$$6P:(DE-H253)PIP1085616$$aMax Planck Institute for Chemical Energy Conversion$$b2
000481804 9101_ $$0I:(DE-HGF)0$$6P:(DE-HGF)0$$aTechnische Universität Berlin$$b3
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000481804 9101_ $$0I:(DE-HGF)0$$6P:(DE-HGF)0$$aHumboldt-Universität zu Berlin$$b5
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000481804 9101_ $$0I:(DE-HGF)0$$6P:(DE-HGF)0$$aHumboldt-Universität zu Berlin$$b11
000481804 9101_ $$0I:(DE-HGF)0$$6P:(DE-H253)PIP1015325$$aMax Planck Institute for Chemical Energy Conversion$$b12
000481804 9101_ $$0I:(DE-HGF)0$$6P:(DE-H253)PIP1100480$$aTechnische Universität Berlin$$b13
000481804 9101_ $$0I:(DE-HGF)0$$6P:(DE-HGF)0$$aTechnische Universität Berlin$$b14
000481804 9101_ $$0I:(DE-HGF)0$$6P:(DE-HGF)0$$aTechnische Universität Berlin$$b15
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000481804 9141_ $$y2022
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