Notes: Eicosanoids and Related Lipid Mediators

Eicosanoids: Overview and Key Topics

  • Eicosanoids are a class of molecules derived from 20-carbon polyunsaturated fatty acids, most frequently arachidonic acid. They act on the cells that produce them or on neighboring cells, and are therefore autocrine/paracrine hormones that are very quickly metabolized.

  • Major topics covered: structure of eicosanoids; pathways by which they are synthesized; cellular receptors and biological activity; current areas of clinical importance; clinically important inhibitors of eicosanoid synthesis; specialized pro-resolving mediators (SPMs) as a new class of lipid-based inflammatory regulators.

Lipids: General properties and biological functions

  • Lipids are structurally diverse organic molecules characterized by low solubility in water and relatively hydrophobic nature.

  • Biological functions include storage of energy (reduced compounds; high energy density; good packing), insulation from environment (low thermal conductivity; high heat capacity), mechanical protection (shock absorption), water repellency (prevents wetting and minimizes water loss via evaporation).

  • Membrane structure: lipids form the main structure of cell membranes.

  • Cofactors for enzymes: Vitamin K (blood clot formation) and Coenzyme Q (ATP synthesis in mitochondria).

  • Signaling molecules: autocrine/paracrine hormones (act locally), steroid hormones (act body-wide), growth factors, vitamins A and D (hormone precursors).

  • Pigments: contribute to color in tomatoes, carrots, pumpkins, and some birds.

Eicosanoids: Definition and classification

  • Eicosanoids are a class of molecules derived from 20-carbon (2020-carbon) polyunsaturated fatty acids; the most common substrate is arachidonic acid.

  • They can act on producing cells or adjacent cells, classifying them as autocrine/paracrine hormones that are rapidly metabolized.

  • Key oxidation products include prostaglandins, thromboxanes, and leukotrienes.

Arachidonic Acid Derivatives as Signaling Lipids

  • Enzymatic oxidation of arachidonic acid yields:

    • Prostaglandins (inflammation and fever)

    • Thromboxanes (formation of blood clots)

    • Leukotrienes (smooth muscle contraction in lungs)

  • Core signaling framework involves cyclooxygenase (COX) and lipoxygenase (LOX) pathways leading to various bioactive lipids.

Phospholipids, Phospholipases, and the Release of Arachidonic Acid

  • Cellular membranes contain glycerophospholipids; phospholipases hydrolyze phospholipids to release fatty acids like arachidonic acid.

  • Specific phospholipases:

    • Phospholipase A₁

    • Phospholipase A₂ (PLA₂)

    • Phospholipase C (PLC)

    • Phospholipase D (PLD)

  • Visualization (lipid scaffold): glycerophospholipids in membranes (cellular membrane, nuclear envelope, endoplasmic reticulum) with fatty acids attached to glycerol backbone; hydrolysis releases arachidonic acid.

  • Schematic notes: PLA₂ hydrolyzes the sn-2 position to release arachidonic acid for downstream eicosanoid synthesis.

Specificities of Phospholipases

-PLA₁ and PLA₂ cleave at different sn-positions of phospholipids; PLC cleaves the phosphodiester bond to generate diacylglycerol (DAG) and inositol triphosphate (IP₃); PLD hydrolyzes phosphatidylcholine to produce phosphatidic acid and choline.

  • Important enzyme for arachidonic acid release: PLA₂ activity is a rate-limiting step for eicosanoid biosynthesis.

PLA₂ Isoforms

  • Secreted PLA₂ (sPLA₂): found in venoms of snakes and in mammalian pancreatic enzymes.

  • Cytosolic PLA₂ (cPLA₂): catalyzes the release of arachidonic acid from intracellular membrane phospholipids.

Eicosanoid Biosynthesis: Core Pathways

  • Arachidonic acid is liberated from membrane phospholipids and serves as the substrate for two main enzymatic pathways:

    • Cyclooxygenase (COX) pathway → Prostaglandins, Thromboxanes

    • Lipoxygenase (LOX) pathway → Leukotrienes and related metabolites

  • Central steps include:

    • COX-1/COX-2 generate PGH₂ from arachidonic acid via the cyclooxygenase and peroxidase activities; PGH₂ is the common precursor for prostaglandins (PGE₂, PGD₂, PGF₂α, PGI₂) and thromboxane A₂ (TXA₂).

    • 5-LOX (with 5-LOX-activating protein, FLAP) converts arachidonic acid to leukotriene pathways, ultimately producing LTC₄, LTD₄, LTE₄, and LTB₄.

  • Abbreviations: LOX = lipoxygenase; HPETE = hydroperoxyeicosatetraenoic acid; COX = cyclooxygenase; PG = prostaglandin; TX = thromboxane; LT = leukotriene.

Activation of Phospholipase A₂

  • PLA₂ activation involves receptor-mediated signaling and calcium flux:

    • Ligand binds receptor on the plasma membrane → PLC activation → DAG and IP₃ production.

    • IP₃ elevates cytosolic Ca²⁺; DAG activates PKC; ER Ca²⁺ stores release occurs via IP₃ receptor channels.

    • This Ca²⁺/PKC signaling promotes cPLA₂ activation and translocation to membranes, enabling arachidonic acid release and subsequent COX/LOX metabolism.

  • Downstream products include COX-derived prostaglandins and LOX-derived leukotrienes.

Prostaglandin H Synthase / Cyclooxygenase (COX)

  • COX catalyzes two sequential reactions on arachidonic acid:

    • Cyclooxygenase reaction: incorporation of two O₂ molecules to form PGG₂.

    • Peroxidase reaction: reduction of PGG₂ to PGH₂.

  • Two COX isoforms exist: COX-1 and COX-2, encoded by separate genes; they share about 65%65\% amino acid identity.

  • Structural and functional differences between COX-1 and COX-2 are exploited to develop isoform-specific drugs that limit arachidonic acid access to the active site.

COX-1 vs COX-2: Physiologic vs Inflammatory Roles

  • COX-1 (constitutive):

    • Essential for thromboxane formation in platelets; maintains GI epithelial integrity; renal function; vasodilation; inhibits platelet aggregation; GI mucosal protection and ulcer healing.

  • COX-2 (inducible):

    • Upregulated in inflammatory diseases (arthritis, cardiometabolic diseases); increases prostaglandin production; contributes to angiogenesis via VEGF; may support tumor growth.

  • Overall consequence: COX-2 induction shifts mediator production toward prostaglandins during inflammation vs COX-1–mediated protective roles.

Lipoxygenase and Leukotriene Pathway

  • 5-LOX initiates leukotriene synthesis; requires FLAP for activity; activity is Ca²⁺- and phosphorylation-regulated similar to PLA₂; high LTA₄ levels can inhibit LOX activity (feedback).

  • Leukotrienes (LTs) act through specific GPCRs on leukocytes and other tissues, mediating inflammation and bronchoconstriction in asthma.

Eicosanoid Receptors and Signaling

  • Prostaglandin receptors:

    • PGE₂: EP1, EP2, EP3, EP4

    • PGI₂: IP

    • PGD₂: DP1, DP2

    • PGF₂α: FP

    • TXA₂: TP

  • Signaling cascades (representative):

    • EP receptors couple to Gs or Gi proteins, modulating cAMP and Ca²⁺ signaling; IP, FP, DP1/DP2, TP show various coupling patterns (Gs or Gi) affecting IP₃/Ca²⁺ and cAMP levels.

  • Leukotriene receptors:

    • LTB₄: BLT1, BLT2

    • LTC₄, LTD₄, LTE₄: CysLT₁ and CysLT₂

  • Cellular localization of receptors includes leukocytes, smooth muscle cells, endothelial cells, etc.

  • Signaling outcomes include increased or decreased CAMP, Ca²⁺, IP₃/Ca²⁺, and downstream effects on inflammation and smooth muscle tone.

Biological Actions of Eicosanoids by Tissue

  • Table-style overview (selected examples):

    • Hypothalamus-pituitary axis: PGE₂, PGE₁ regulate hormone secretion, ovulation, luteolysis, implantation.

    • Ovary: PGE₂; PGF₂α involved in reproductive processes.

    • Uterus: PGI₂, PGE₂, PGF₂α regulate contraction and blood flow.

    • Kidney: PGH₂, PGE₁, PGI₂ influence filtration and renal function.

    • Stomach: PGE₂, PGI₂ reduce gastric acid secretion (cytoprotection).

    • Intestine: PGE₁, PGF₂α influence motility.

    • Bronchi: PGE₂, PGI₂ cause bronchodilation; PGF₂α, TXA₂, LTC₄, LTD₄ can cause bronchoconstriction.

  • This section highlights the diverse, tissue-specific actions of prostaglandins, thromboxanes, and leukotrienes in physiological regulation and disease states.

Prostaglandins: Specific Biochemical and Physiological Actions

  • Prostaglandin D₂ (PGD₂): weak inhibitor of platelet aggregation.

  • Prostaglandin E₁ (PGE₁):

    • Bronchial vasodilation

    • Inhibits lipolysis

    • Inhibits platelet aggregation

    • Contraction of gastrointestinal smooth muscle

  • Prostaglandin E₂ (PGE₂):

    • Renal and bronchial vasodilation

    • Stimulates hyperalgesic response (sensitizes-to-pain)

    • Inhibits platelet aggregation

    • Stimulates uterine smooth muscle relaxation

    • Cytoprotection: protects GI epithelium from acid degradation

    • Reduces gastric acid secretion

    • Elevates thermoregulatory set-point in the anterior hypothalamus (fever)

    • Promotes inflammation

  • Prostaglandin F₂α (PGF₂α):

    • Stimulates uterine smooth muscle contraction (note: transcript lists relaxation; canonical physiology often indicates contraction; follow course material as presented)

Prostaglandin I₂ vs Thromboxane A₂

  • PGI₂ (prostacyclin):

    • Potent inhibitor of platelet aggregation; vasodilation; uterine relaxation; can sensitize/amplify nerve pain.

  • TXA₂ (thromboxane A₂):

    • Potent inducer of platelet aggregation; vasoconstriction (including bronchioles, renal vasculature); decreases (reduces) cAMP in platelets; stimulates release of ADP and 5-HT from platelets.

  • Clinical note: Aspirin is commonly used for anti-clotting effects due to inhibition of TXA₂ formation in platelets.

Leukotrienes: Functions and Disease associations

  • Synthesis: 5-LOX (with FLAP) converts arachidonic acid to leukotrienes.

  • Primary actions: chemotaxis and activation of neutrophils; recruitment and activation of eosinophils; bronchoconstriction in asthma; increased vascular permeability and mucus production.

  • Receptors and signaling:

    • LTB₄ via BLT1/BLT2 receptors mediates neutrophil activity and chemotaxis.

    • CysLTs (LTC₄, LTD₄, LTE₄) via CysLT₁ and CysLT₂ receptors mediate bronchoconstriction and vascular effects.

  • Disease associations (examples): arthritis, atherosclerosis, cancer, dermatitis, COPD, inflammatory bowel disease (IBD), asthma, allergic rhinitis, aortic aneurysm, ischemia/stroke.

  • Leukotriene pathway inhibitors used clinically include 5-LOX inhibitors and leukotriene receptor antagonists.

Inhibitors of Eicosanoid Synthesis and Action

  • Eicosanoid inhibitors fall into two main classes:

    • Corticosteroids (glucocorticoids): inhibit PLA₂, reducing arachidonic acid availability for COX and LOX, thereby suppressing production of all eicosanoids; broad anti-inflammatory effects but with significant long-term side effects.

    • Nonsteroidal anti-inflammatory drugs (NSAIDs): COX inhibitors; block prostaglandin and thromboxane synthesis by inhibiting COX (prostaglandin H₂ synthase).

    • Aspirin (Acetylsalicylate): irreversible inhibitor; acetylates a serine residue in the COX active site; inhibits COX-1 and COX-2.

    • Ibuprofen and naproxen: competitive inhibitors; resemble substrate and inhibit COX-1 and COX-2.

  • Other COX/LOX targeted agents:

    • Zileuton: 5-LOX inhibitor.

    • Zafirlukast and Montelukast: leukotriene receptor antagonists targeting CysLT receptors.

Side Effects and Clinical Considerations of NSAIDs

  • Side effects arise from broad COX inhibition across tissues:

    • Gastrointestinal system: risk of ulcers and bleeding; major limitation for chronic use.

    • Kidney and liver toxicity risk.

  • COX-2 inhibitors (e.g., Vioxx, Bextra, Celecoxib) were developed to reduce GI toxicity but have their own risks.

    • Some COX-2 inhibitors were withdrawn due to increased thrombotic and cardiovascular events; disruption of balance between PGI₂ (vasodilation, platelet inhibition) and TXA₂ (vasoconstriction, platelet aggregation).

  • NSAIDs can shift arachidonic acid metabolism toward leukotriene production, potentially worsening asthma symptoms in susceptible individuals.

Summary Diagram: Phospholipid Arachidonic Acid Pathway to Eicosanoids

  • Substrate pool: Phospholipids containing arachidonic acid undergo PLA₂ action to release arachidonic acid.

  • COX pathway: Arachidonic acid → PGG₂ (cyclooxygenase) → PGH₂ (peroxidase) → downstream prostaglandins (PGE₂, PGD₂, PGF₂α, PGI₂) and TXA₂ via respective synthases.

  • LOX pathway: Arachidonic acid → HPETE via LOX; further metabolism yields leukotrienes (LTB₄, LTC₄, LTD₄, LTE₄).

  • Inhibitors target: PLA₂ (corticosteroids), COX (NSAIDs), 5-LOX (Zileuton), leukotriene receptors (Zafirlukast, Montelukast).

  • Receptor signaling: Prostaglandins and leukotrienes exert their actions through specific GPCRs (EP, IP, FP, DP, TP; BLT and CysLT receptors).

Specialized Pro-resolving Mediators (SPMs): A New Class of Lipid Inflammatory Regulators

  • Concept: Resolution of inflammation is an active, biosynthetic process mediated by SPMs.

  • Four major classes:

    • Resolvins

    • Lipoxins

    • Protectins

    • Maresins

  • Biosynthesis:

    • SPMs derive from fatty acids such as arachidonic acid (AA), eicosapentaenoic acid (EPA), and docosahexaenoic acid (DHA).

    • Enzymes involved include COX-1/COX-2, LOX, and cytochrome P450 pathways; aspirin can acetylate COX-2 to generate aspirin-triggered SPMs.

  • Functional role: active resolution of inflammation, promoting clearance of microbes, reducing pain, and enhancing tissue regeneration via specific cellular and molecular mechanisms.

  • Representative SPMs and examples:

    • Lipoxins (e.g., Lipoxin A₄, LXA₄)

    • E-series resolvins (e.g., Resolvin E1, RvE1) derived from EPA

    • D-series resolvins (e.g., Resolvin D1, RvD1) derived from DHA

    • Protectins (e.g., Protectin D1, PD1)

    • Maresins (e.g., Maresin 1, MaR1)

  • Important nuance: Anti-inflammatory is not identical to pro-resolution; SPMs actively drive resolution, including microbe clearance and tissue repair.

Selected Contemporary Literature and Context (examples from provided sources)

  • Recent reviews and mini-reviews summarize the roles of eicosanoids in cardiovascular health, rheumatoid arthritis, NAFLD, and COVID-19-related inflammation resolution.

    • Eicosanoids in atherosclerosis and cardiometabolic health (Piper & Garelnabi).

    • Systematic reviews on eicosanoid pathways in rheumatoid arthritis.

    • Eicosanoids in NAFLD progression and serum eicosanoid profiles.

    • Inflammation resolution as a dual-pronged approach to cytokine storms in COVID-19.

  • These sources illustrate the broad relevance of eicosanoids across physiology, pathology, and emerging therapeutic strategies focused on resolution of inflammation.

Practical Implications and Takeaways

  • Therapeutic strategies target different nodes of the eicosanoid network:

    • Antiinflammatory effects via corticosteroids (PLA₂ inhibition) or NSAIDs (COX inhibition).

    • Targeted leukotriene pathway blockade in asthma (5-LOX inhibitors, leukotriene receptor antagonists).

    • Consideration of cardiovascular risks with COX-2 inhibitors and the balance between PGI₂ and TXA₂.

    • Emergence of SPMs as therapies to actively promote resolution rather than simply suppress inflammation.

  • The choice of inhibitor (COX-1 vs COX-2 selectivity, reversible vs irreversible inhibition) has tissue-specific and systemic consequences, including GI, renal, and cardiovascular safety profiles.

Key Formulas and Notations

  • Prostaglandin and thromboxane synthesis (simplified):

    • Arachidonic acid
      extArachidonicacid<br>ightarrowextPGG<em>2ightarrowextPGH</em>2ext{Arachidonic acid} <br>ightarrow ext{PGG}<em>2 ightarrow ext{PGH}</em>2 via COX-1/COX-2;

    • PGH₂ then converted to downstream prostaglandins (PGE₂, PGD₂, PGF₂α, PGI₂) and TXA₂ via specific synthases.

  • Leukotriene synthesis:

    • Arachidonic acid → HPETE via 5-LOX (with FLAP) → LTA₄ → LTD₄/LTE₄ and LTB₄ through subsequent enzymatic steps.

  • Receptor signaling examples:

    • EP receptors (PGE₂) couple to Gs or Gi; IP couples to Gs; FP, DP1/DP2, and TP have receptor-specific signaling.

    • BLT receptors for LTB₄ (BLT1/BLT2) and CysLT receptors (CysLT₁/CysLT₂) for LTC₄/LTD₄/LTE₄.

  • Inhibitors and targets:

    • COX inhibition reduces production of all COX-derived prostaglandins and TXA₂.

    • 5-LOX inhibition reduces leukotriene production.

    • Leukotriene receptor antagonists block LT signaling at the receptor level.

Key Quick References (to recall during exams)

  • COX-1: constitutive; GI mucosa protection; thromboxane production in platelets.

  • COX-2: inducible; upregulated in inflammation; angiogenesis via VEGF; associated with inflammatory diseases.

  • PGE₂: pro-inflammatory mediator; fever; pain sensitization; renal and bronchial vasodilation; cytoprotection in GI tract.

  • PGI₂ vs TXA₂: PGI₂ inhibits platelet aggregation and causes vasodilation; TXA₂ promotes platelet aggregation and vasoconstriction; balance is clinically important.

  • Leukotrienes: key players in asthma and bronchoconstriction; BLT and CysLT receptors mediate their effects.

  • SPMS: actively resolve inflammation; four classes with EPA/DHA/AA substrates; aspirin can trigger certain SPMs; promote healing and reduce pain.