bioRxiv Science⌕ Search

Biology subjects

Kreiter, J.

Publications and source records attributed to Kreiter, J..

5 recordsLinked to original sources

Mechanism of Gating and Isoform-Specific Inhibition in Renal CLC Chloride Channels

Hyponatremia is a prevalent disorder marked by excess water retention and substantial morbidity, motivating interest in the CLC-Ka chloride channel as a therapeutic target. Selectively inhibiting CLC-Ka without affecting the closely related CLC-Kb is essential for preventing serious side effects. However, developing isoform-selective inhibitors has been challenging because most small molecules do not distinguish between CLC-Ka and CLC-Kb, and the basis for selectivity in the few known exceptions remains unclear. The small molecule BIM1 preferentially inhibits CLC-Ka over CLC-Kb, providing an opportunity to dissect isoform-specific pharmacology. To investigate this mechanism, we determined cryo-EM structures of BIM1 and BIM15, a related nonselective analog, bound to a CLC-K variant engineered to match the human CLC-Ka binding pocket. Structural and computational analyses reveal that inhibition and isoform selectivity are anchored by interactions with a conserved lysine, with surrounding binding-site residues subtly tuning the local electrostatic environment to promote or disfavor these contacts. These analyses further identify a dynamic extracellular loop that intermittently occludes the shared pathway accessing the inhibitor-binding site and pore. Bound BIM15 engages this gating loop more extensively than BIM1, suggesting that differential loop engagement contributes to inhibitor selectivity, a prediction validated by mutagenesis. Because loop dynamics block the pore, we examined the structural impact of Ca{superscript 2}, which favors opening, and found the gating loop ordered and withdrawn from the pathway. Together, these findings define how binding-site microenvironments and gating-loop dynamics shape isoform-specific inhibition and pore access in CLC-K channels. Significance StatementHyponatremia is a major clinical problem with limited therapeutic options. The kidney chloride channel CLC-Ka is an attractive drug target, but its high sequence identity to CLC-Kb has hindered the development of isoform-selective inhibitors needed for safe therapy. A low-micromolar CLC-Ka-selective inhibitor had been identified, providing a foothold for drug development, but the structural basis of its selectivity was unknown. Here, by integrating cryo-EM structures with molecular dynamics simulations, we define the inhibitor-binding site and reveal the mechanism that enables preferential CLC-Ka inhibition. We further show that a dynamic extracellular loop functions as a gating element shaping inhibitor access and engagement. These findings establish a mechanistic foundation for developing improved treatments for hyponatremia.

biophysics↗

Molecular mechanism of exchange coupling in CLC chloride/proton antiporters

The ubiquitous CLC membrane transporters are unique in their ability to exchange anions for cations. Despite extensive study, there is no mechanistic model that fully explains their 2:1 Cl-/H+ stoichiometric exchange mechanism. Here, we provide such a model. Using differential hydrogen-deuterium exchange mass spectrometry, cryo-EM structure determination, and molecular dynamics simulations, we uncovered conformational dynamics in CLC-ec1, a bacterial CLC homolog that has served as a paradigm for this family of transporters. Simulations based on a cryo-EM structure at pH 3 revealed critical steps in the transport mechanism, including release of Cl- ions to the extracellular side, opening of the inner gate, and water wires that facilitate H+ transport. Surprisingly, these water wires occurred independently of Cl-binding, prompting us to reassess the relationship between Cl- binding and Cl-/H+ coupling. Using isothermal titration calorimetry and quantitative flux assays on mutants with reduced Cl- binding affinity, we conclude that, while Cl- binding is necessary for coupling, even weak binding can support Cl-/H+ coupling. By integrating our findings with existing literature, we establish a complete and efficient CLC 2:1 Cl-/H+ exchange mechanism.

biophysics↗

The non-thermogenic function of opossum UCP1 is independent of its cytoplasmic binding network.

The primary function of uncoupling protein 1 (UCP1) is to mediate non-shivering thermogenesis in brown adipose tissue by facilitating proton transport across mitochondrial membranes. However, recent study has shown that UCP1 from the opossum (a marsupial) lacks thermogenic activity (Keipert et al., Science, 2024). This deficiency was attributed to two altered residues, K100 and Y289, within the cytosolic salt bridge network. Interestingly, the same residues are also present in UCP2 and UCP3 from murine species, both of which are known to transport protons in the presence of long-chain fatty acids (FAs). This raises questions about the validity of the proposed mechanism involving these residues in the loss of thermogenic function in opossum UCP1. In this study, we performed conductance measurements of planar lipid bilayers reconstituted with either recombinant mouse UCP1, or UCP1 mutant (Q100K/F289Y), or UCP2, or UCP3. Our data demonstrate that the conductance of the UCP1 double mutant, UCP2, and UCP3 is comparable to that of wild-type mouse UCP1 in the presence of palmitic or arachidonic acids. These findings suggest that the altered cytosolic residues (K100 and Y289) do not explain the lack of thermogenic function in opossum UCP1. Thus, the underlying molecular mechanism responsible for the absence of thermogenesis in opossum UCP1 remains unresolved, and further studies are warranted to elucidate the precise cause of this dysfunction. Given the emerging interest in UCP1 uncoupling as a potential therapeutic approach for treating obesity by increasing energy expenditure, understanding the molecular basis of UCP1s thermogenic dysfunction is of significant relevance.

biophysics↗

The 2-oxoglutarate/malate carrier extends the family of mitochondrial carriers capable of FA-activated proton transport.

Metabolic reprogramming in cancer cells has been linked to the mitochondrial dysfunction. Recent studies have suggested the mitochondrial 2-oxoglutarate/malate carrier (OGC) as a potential target for preventing cancer progression. Although OGC is known to be a part of the malate/aspartate shuttle, its exact role in cancer metabolism remains unclear. In this study, we investigated the contribution of recombinant murine OGC to the proton transport by measuring the conductance (Gm) of planar lipid bilayer membranes reconstituted with OGC. Our results show that OGC significantly increases Gm only in the presence of free fatty acids (FAs) and 2,4-dinitrophenol, demonstrating for the first time its involvement in proton transport. We found that (i) the increase in OGC activity directly correlates with the increase in the number of unsaturated bonds of FAs, and (ii) OGC substrates and inhibitors compete with FAs for the same binding site. In addition, we have identified R90 as a crucial amino acid of the binding site for FAs, ATP, 2-oxoglutarate, and malate, which is a first step towards understanding the OGC-mediated proton transport mechanism. Elucidating the contribution of OGC to the uncoupling will be crucial in the design of targeted drugs for the treatment of cancer and other metabolic diseases.

biophysics↗

Mechanism of the ANT-mediated transport of fatty acid anions across the inner mitochondrial membrane

The additional protonophoric function of the mitochondrial adenine nucleotide translocase (ANT1) is now recognized. However, the molecular mechanism remains controversial. Fatty acid (FA) cycling hypothesis postulates that FAs transport protons across the inner mitochondrial membrane to the matrix by a flip-flop, whereas ANT1 facilitates the translocation of FA anions (FA-) back to the intermembrane space. By a combined approach involving measurements of current through the planar lipid bilayers reconstituted with recombinant ANT1, site-directed mutagenesis and molecular dynamics simulations, we show that FA- is initially caught by R59 on the matrix side of ANT1, then moves along the positively charged protein-lipid interface, and binds to R79, where it is protonated in the hydrated cavity in the presence of D134. R79 is crucial for the competitive binding of ANT1 substrates (ATP and ADP) and inhibitors (carboxyatractyloside, bongkrekic acid). The binding sites are well-conserved in mitochondrial SLC25 members, implying a general transporting mechanism for FA anions.

biophysics↗