Leibniz-Institute for Food Systems Biology, Technical University of Munich, Lise-Meitner-Str. 34, 85354, Freising, Germany.
Department of Chemistry, Yale University, New Haven, CT, 06520, USA.
Cell Mol Life Sci. 2020 Jun;77(11):2157-2179. doi: 10.1007/s00018-019-03279-y. Epub 2019 Aug 21.
Sulfur-containing compounds within a physiological relevant, natural odor space, such as the key food odorants, typically constitute the group of volatiles with the lowest odor thresholds. The observation that certain metals, such as copper, potentiate the smell of sulfur-containing, metal-coordinating odorants led to the hypothesis that their cognate receptors are metalloproteins. However, experimental evidence is sparse-so far, only one human odorant receptor, OR2T11, and a few mouse receptors, have been reported to be activated by sulfur-containing odorants in a copper-dependent way, while the activation of other receptors by sulfur-containing odorants did not depend on the presence of metals. Here we identified an evolutionary conserved putative copper interaction motif CC/CSSH, comprising two copper-binding sites in TMH5 and TMH6, together with the binding pocket for 3-mercapto-2-methylpentan-1-ol in the narrowly tuned human receptor OR2M3. To characterize the copper-binding motif, we combined homology modeling, docking studies, site-directed mutagenesis, and functional expression of recombinant ORs in a cell-based, real-time luminescence assay. Ligand activation of OR2M3 was potentiated in the presence of copper. This effect of copper was mimicked by ionic and colloidal silver. In two broadly tuned receptors, OR1A1 and OR2W1, which did not reveal a putative copper interaction motif, activation by their most potent, sulfur-containing key food odorants did not depend on the presence of copper. Our results suggest a highly conserved putative copper-binding motif to be necessary for a copper-modulated and thiol-specific function of members from three subfamilies of family 2 ORs.
在生理相关的自然气味空间中,含硫化合物,如关键的食物气味剂,通常构成挥发性最低气味阈值的化合物组。某些金属(如铜)增强含硫金属配位气味剂的气味的观察结果导致了这样的假设,即它们的同源受体是金属蛋白。然而,实验证据很少——到目前为止,只有一种人类气味受体 OR2T11 和几种小鼠受体被报道以铜依赖的方式被含硫气味剂激活,而其他受体被含硫气味剂的激活不依赖于金属的存在。在这里,我们鉴定了一个进化保守的假定铜相互作用基序 CC/CSSH,它由 TMH5 和 TMH6 中的两个铜结合位点以及在高度调谐的人类受体 OR2M3 中 3-巯基-2-甲基戊烷-1-醇的结合口袋组成。为了表征铜结合基序,我们将同源建模、对接研究、定点突变和重组 OR 在基于细胞的实时发光测定中的功能表达结合起来。OR2M3 的配体激活在铜存在下增强。这种铜的作用被离子和胶体银模拟。在两个广泛调谐的受体 OR1A1 和 OR2W1 中,没有发现假定的铜相互作用基序,它们最有效的含硫关键食物气味剂的激活不依赖于铜的存在。我们的结果表明,一个高度保守的假定铜结合基序对于家族 2 OR 三个亚家族成员的铜调节和硫醇特异性功能是必要的。