Concept of Free Energy

 Concept of Free Energy

Definition – Free energy is that portion of the energy of a system available to do work as the system proceeds toward equilibrium under conditions of constant temperature and pressure and volume The change in free energy content (ΔG) depends on two components ΔH (change in enthalpy, internal energy heat) and ΔS (change in entropy)
Chemical reaction performs work if it can be harnessed in utilizable form of energy. Amount of work performed depends on the efficiency of the machinery. 
Free energy change of a biological reactions is reported as the standard free energy change (ΔG0’) 
ΔG0’- is the value of ΔG for a reaction at standard conditions for biological reactions (pH 7, 1M, 25o C, 1 atmosphere pressure) 
Free energy change is used to predict the direction and equilibrium of chemical reactions If ΔG is negative – net loss of energy (exergonic) 
 - reaction goes spontaneously 
If ΔG is positive - net gain of energy (endergonic) reaction does not go spontaneously 
If ΔG is zero- reactants are in equilibrium 

C - Oxidation-Reduction Reactions 

The utilization of chemical energy in living system involves oxidation – reduction reactions. For example, the energy of chemical bonds of carbohydrates, lipids and proteins is released and captured in utilization form by processes involving oxidation- reductions. I- Oxidation - removal of electron(s) from substance - usually accompanied by a decrease in energy content of oxidized substance II-Reduction - addition of electron(s) to a substance usually accompanied by an increase in energy content of reduced substance Oxidation reduction reactions are coupled processes 

III- Reduction Potential (Oxidation-reduction potential, E'o )

-Concept Definition - Measure of electron donating tendencies Electrically measured in reference to a standard substance H2. Determined by measuring the electromotive force generated by a sample half-cell with respect to standard reference halfcell Anegative E’o = lower affinity for electrons A positive E’o = higher affinity for electrons 
In this example, 2H+ /H2 redox pair has negative E’o - Electron donating tendency where as ½ O2/H2O redox pair has positive E’o - Electron accepting tendency Hence, H2 - electron donor (oxidized) O2 - electron acceptor (reduced)
Most molecules serve as both electron donors and electron acceptors of different times depending upon what other substances they react with. In biological systems the primary electron donors are fuel molecules such as carbohydrates, fats and proteins. The oxidation of these substances transfers electrons to intermediate electron carriers such as NAD+ , NADP+ and FAD to reduce them to their reduced state NADH, and FADH2. Reduction potential of the NAD+ / NADH pair is – 0.32Volt, placed high on the electron tower, good electron donor and that of ½ O2 /H2O is +0.82volts. 

In respiratory chain the electrons from NADH are transferred through a series of carriers (organic or inorganic) until they are accepted by molecular oxygen (O2) releasing energy at different levels. The free-energy change of an oxidation – reduction reaction can be calculated from the difference in reduction potentials of the reactants using the formula:  
Under cellular condition part of the free-energy of oxidation of reducing equivalents is conserved in the form of high-energy phosphate compound, ATP. This occurs by the help of energy conserving system in the inner mitochondrial membrane of eukaryotes or plasma membrane of prokaryotes.
 Fig 3.2. Change in free energy as a result of oxidation of NADH

Aerobic Energy-Generation 

In aerobic organisms the complete breakdown of fuel molecules, carbohydrates, fats and proteins takes place in mitochondria of eukaryotes and cytoplasmic membrane and cytoplasm of aerobic prokaryotes. The fuel molecules are metabolized to a common intermediate called aceyl CoA which is further degraded by a common pathway called Kreb’s cycle. This metabolic pathway in addition to providing energy provides building blocks required for growth, reproduction, repair and maintenance of cellular viability. 

Mitochondria 

- it is an organelle where major amount of energy produced. Structurally it is bounded by two separate membranes (outer mitochondrial membrane and inner mitochondrial membrane) 

Out membrane 
- smooth and unfolded 
- Freely permeable to most ions and polar molecules (Contain porous channels) 

Inner membrane 
- folded into cristae-increased surface area 
- Highly impermeable to most ions and polar molecules 

Contain transporters which access polar and ionic molecules in and out Cristae are characteristic of muscle and other metabolically active cell types 
- Protein-rich membrane (about 75%)

 Inter membrane space – space between outer and inner membranes Matrix-the internal compartment containing soluble enzymes and mitochondrial genetic material

Oxidation of Pyruvate 

Pyruvate is common intermediate of many catabolic reactions. It is still energy rich molecule. It is a cross road molecule which can be converted into different intermediates depending on :- type of cells-eukaryotes except RBC- acetyl CoA 
- aerobic prokaryotes- acetyl CoA 
- anaerobic prokaryotes- ethanol or lactate 
- in RBC-always lactate 
absence or presence of oxygen -lactate, ethanol or acetyl-CoA 
- high ratio of NADH/NAD+ favors lactate formation in actively exercising muscle (oxygen limitation) 
Oxidation of pyruvate into acetyl CoA-aerobic process (O2 terminal electron-acceptor) which takes place in the mitochondrial matrix of eukaryotic cells Pyruvate is transported into mitochondrial matrix by special transporter.Inside matrix pyruvate is oxidized into acetylCoA by pyruvate dehydrogenase complex which is complex of E1, E2 and E3 enzymes.This enzyme requires s five coenzymes- TPP, Lipoate, CoA, FAD and NAD+ 
Where:
E1 = pyruvate dehydrogenase, 
E2 = dihydrolipoyl transacetylase, 
E3 = dihydrolipoyl dehydrogenase
Regulation of Pyruvate Dehydrogenase 
Product Inhibition by 
- acetyCoA 
 - elevated levels of NADH 
Covalent modification - dephosphorylated (active) - Increased ADP/ATP ratio 
- Phosphorylated (inactive) - increased acetylCoA/CoA ratio 
 - Ncreased NADH/NAD+ ratio

KREB’S CYCLE 

Also called-tricarboxylic acid cycle (TCA) or Citric acid cycle Final common pathway for complete exudation of carbohydrates, fatty acids and many amino acids.Common pathway for catabolism of acetyl COA ,a common intermediate of different catabolic pathways  

Aerobic process (occurs in aerobic cells in presence of oxygen (O2). Reactions take place in cytosol of prokaryotes and mitochondria matrix of eukaryotes
Fig 3.4 The citric acid cycle

Reactions of Kreb’s cycle 

1. Condensation of acetyl COA with oxaloacetate by citrate synthase (condensing enzyme) to form citrate. 
Considerable free energy is lost as heat due to hydrolysis of thisester bond (drive the reaction forward). 

2. Isomerization of citrate to isocitrate by aconitase 

Aconitase contains iron - sulfer (Fe:S) cluster that assists the enzymatic activity fluoroacetate (potent rodenticide) inhibits aconitase with the ultimate effect of blocking Kreb’s cycle and oxidative phosphorylation.

3. Oxidative decarboxylation of isocitrate by isocitrate dehydrogenase 
There are three types of isocitrate dehydrogenases NAD+ - specific – only mitochondrial NADP+ - specific – cytosolic and mitochondrial Respiratory chain linked oxidation of isocitrate proceeds almost completely through NAD+ - dependent enzyme * Cytosolic isocitrate dehydragenase reaction generates NADPH and CO2 anabolic role 

4. Oxidative decarboxylation of α- ketoglutarate by α - ketoglutarate dehydrogenase complex 
α-ketoglutarate is structurally and functionally similar to pyruvate dehydrogenase complex of three enzymes (A’ B’ C’)
A’ (α - ketoglutarate dehydrogenase), B’ (transuccinylase), C’ (dihydrolipoyl dehydrogenase). This enzyme has the same coenzyme requirement to that of pyruvate dehydrogenase complex. The reaction releases considerable energy, part of which is used to form high-energy thioester bond and NADH. Arsenite inhibits α-Ketoglutarate dehydrogenese complex blocking Kreb’s cycle. α-Ketoglutarate accumulates upon poisoning of the enzyme. Arsenite is also inhibitor of pyruvate dehydrogenase complex 

5. Conversion of succinyl CoA into succinate by succinate thiokinase (succinyl CoA synthetase) 
GTP is formed by substrate – level phosphorylation Fates of GTP - participate in mitochondrial protein synthesis Converted into ATP.

6. Oxidation of succinate by succinate dehydrogenase 
- Stereospecific for transfer of H-atoms of succinate (*) 
- Succinate dehydrogenese – is integral part of inner mitochondrial membrane 
- Contains Fe – S centers (non-heme iron protein) and FAD as prosthetic groups 
Flavoprotein 
- Inhibited by malonate which competes for the active site of the enzyme 
-OOC-CH2-COO- (Malonate) 
 - Also inhibited by oxaloacetate resulting in succinate accumulation.  

7. Hydration of Fumarate by Fumarase 
- Fumarase is stereospecific for L-malate (catalyzes stereospecific trans addition of H and OH).

8. Oxidation of L-malate by NAD–linked malate dehydrogenase  
This reaction regenerates oxaloacetate, used in the first reaction. N.B: The cycle is aerobic process i.e. regeneration of oxidized coenzymes requires O2 as terminal electron acceptor. No net consumption or production of cycle intermediates Oxaloacetate plays catalytic role in catabolism of acetyl CoA Energy of acetyl CoA catabolism is partly conserved as reducing equivalents (NADH and FADH2) and GTP GTP is formed by substrate – level phosphorylation (synthesis of ATP related to oxidation of substrates not related to electron transport) Net consumption of two molecules of H2O Enzymes – soluble and membrane attached (succinate dehydrogenase)
b-Functions of Kreb’s Cycle Kreb’s cycle has catabolic and anabolic functions Energy generation 
– reducing equivalents,NADH and FADH2 
– TP 
Provide CO2 used for 
– gluconeogenesis 
– fatty acid synthesis 
– urea synthesis 
– ucleotide synthesis 
Provide precursors for 
– gluconeogenesis (all intermediates) 
– amino acid synthesis (non-essial amino acids) – heme synthesis (succinyl CoA) 
– fatty acid synthesis (citrate) 
Regulate other pathways – citrate (inhibit phosphofructokinase) pyruvate carboxylation with formation of oxaloaccetate replenishes the cycle intermediates used for biosynthesis

C - Regulation of Kreb’s Cycle

Primary function of the cycle is to provide energy, thus rate of the cycle is adjusted to meet an animal cells ATP demand. Increased utilization of ATP increases the rate the cycle because of availability of oxidized coenzymes necessary for the continuation of the cycle (NAD+, FAD) and ADP which is needed for oxidative phosphorylation. High levels of ATP and NADH are inhibitory indicating high energy status of the cell. ATP inhibits both citrate synthase and isocitrate dehydrogenase where as both are activated by high levels of ADP. NADH inhibits isocitrate dehydrogenase and α-Ketoglutarate dehydrogenase. Complementary mechanisms of controlling rate of acetyl CoA formation and rate of acetyl CoA degradation is also involved

III- Electron Transport system and Oxidative Phosphorylation 

In aerobic organisms the major amount of ATP is synthesized by phosphorylation of ADP related to electron transport, a process occurring on the inner mitochondrial membrane of eukaryotes. It is a system composed of a chain of membrane associated electron carriers. 

a- Components: 

flavoproteins – FMN and FAD prosthetic groups. Accept H atoms but donate electrons nonheme iron-sulfur proteins (Fe: S centers). Carry electrons not H – atoms. They are component of complexes (I, II and III) Coenzyme Q - Non protein component, Quinone derivative, lipid soluble. Common form in mammals is Q10 Containing ten isoprene units. Accept H – atom but donate electrons. CoQ is mobile carrier of electrons between flavoproteins and cytochromes. Accept electrons from flavoproteins and donate to cytochromes. Transfer and accept two electrons at a time Cytochromes – heme conjugated proteins 
Heme = Fe2+/F3+ + porphyrin
Include classes of cytochromes designated a, b, and c. Iron at the center of cytochromes accept and donates single electron 
Cytochrome with relatively less positive reduction potential (i.e. cyt b) accepts electrons from CoQH2 and transfers them to the next acceptor cytochrome with more positive reduction potential the electron carriers except for CoQ are prosthetic groups of proteins Components of electron transport system are arranged according to the increasing order reduction potentials, a component with more negative reduction potential – at the top component with more positive reduction potential at the bottom. The components of respiratory chain are organized into four complexes and two mobile electron carriers 
Complexes of respiratory chain are designated complex I, II, III and IV (integral parts of inner mitochondrial membrane). CoQ and cytochrome C are mobile electron carriers which act as a link between the complexes. 

Complex                                          Components 
I (NADH dehydrogenase)               FMN, Fe-S centers 
II (Succinate dehydrogenese)          FAD, Fe-S centers 
III (Cytochrome reductase)            cyt.b, cytc, Fe-S center 
IV (Cytochrome oxidase)               cyt.a, cyt.a3 ,copper (Cu1+/Cu2+)  

Table 2. Components of electron transport chain 
Complexes I, III and IC are proton pumps (trans-member and proteins) linked by CoQ and Cyt.c (mobile electron carriers)
b - Oxidation of reducing equivalents (NADH & FADH2) and electron flow through respiratory chain
Complex I 
Electrons from NADH enter at complex I to be relayed to CoQ through series of carriers Q also accepts a pair of electrons from FADH2 prosthetic group of complex II (succinate dehydregenase), glycerol phosphate dehydrogenase (GPDH) and fatty acyl dehydrogenase (FADH) 

Complex IV 
Every step of electron transport in the electron transport chain is accompanied by release of energy Useful energy is captured at three sites because large enough change in free energy (at least 9 - 10 Kcal/mole) occurs at three different sites when electron pairs flow down from NADH to O2. The large enough drop in free energy is occurs when electrons are transferred: within the NADH dehydrogenase complex, from NADH to CoQ, within cytochrome reductase from CoQ to Cyt.c, within cytochrome oxidase from cytc to O2. Such drop in free-energy is more than enough to sponsor the synthesis of three ATP from 3ADP and 3PI 
Flow of a pair of electrons from FDH2 to O2 exhibits only two large drops in free-energy, therefore sponsors the synthesis of only two ATP molecules. That is, the drop in free-energy as electrons pass from FADH2 to CoQ is insufficient to sponsor ATP synthesis. Oxidation of NADH releases more than enough free energy (-52.6kcal) needed for synthesis of 3ATP Similarly oxidation of FADH2 releases more than enough free energy for synthesis of 2ATP.

C- Coupling of Electron Transport and ATP Synthesis (Oxidative Phosphorylation) 

- Electron transport and oxidative phosphorylation are coupled processes Suggested hypotheses for coupling mechanism High-energy intermediate serves as precursor of ATP Activated protein conformation drives the synthesis of ATP Proton gradient across inner mitochondrial membrane couples electron transport and ATP synthesis (chemiosmostic hypothesis of Peter Mitchell- postulated in 1961) Mitchell’s chemiosmotic is the accepted theory According to chemiosmotic theory, electron - transport and oxidative phosphorylation are coupled by proton-gradient as follows. As electrons from NADH or FADH2 flow down the respiratory chain to O2 free energy is released. The free energy released is captured at three sites to pump protons against concentration gradient from matrix to inter membrane space generating proton gradient across inner mitochondrial membrane. As a result of this pH gradient is also formed, more positive (acidic) on the outer side more negative (basic) on the inner side of mitochondria. In this process a proton motive force of 0.22Volts is created across inner mitochondrial membrane. Now the kinetic energy of electrons is transformed into the proton – motive force. This force drives later ATP synthesis This happens when protons are back translocated into matrix through the channel portion of ATP synthase (Fo) which is activated by electrochemical potential difference across the membrane. Catalytic portion of ATP synthase (F1) synthesizes ATP from ADP and Pi as protons are back translocated.  
Fig 3.6. ATP synthesis coupled to electron transport
The precise number of protons pumped by each complex is not known with certainty 
Current estimates 
- 3 - 4 H + by complex I 
- 4 H + by complex II 
- 2 H + by complex IV. 
Under cellular conditions, oxidation of: NADH produces 3ATP from 3ADP and 3PI FADH2 produces 2ATP from 2ADP and 2PI Fates of mitochondrial ATP used by mitochondria energy (ATP) requiring process translocation to cytosol (where most of ATP is used for biosynthesis) by ATP – ADP translocase (antiporter)

d- Respiratory Control 

The most important factor determining the rate of oxidative phosphorylation is the level of ADP which in turn is determined by the rate of ATP consumption cellular energy demand and utilization determines the rate of ATP synthesis through its effect on the level of ADP which controls the rates of oxidative phosphorylation and kreb’s cycle ATP synthesis requires availability of ADP also regeneration of oxidized coenzymes (NAD+ and FAD) required for Kreb’s cycle requires ADP that can be phosphorylated to ATP 

e- Uncoupling of Electron Ttransport and Oxidative Phosphorylation 

Uncouplers are substances which uncouple electron transport and oxidative phosphorylation In the presence of uncouplers: electron transport proceeds proton translocation by proton pumps proceeds oxygen consumption proceeds aerobic oxidations proceed without control Proton gradient is not formed since uncouplers carry protons back to matrix through IMM not through ATP synthase (continuous dissipation of proton – gradient) ATP synthase not activated No ATP synthesis  
Energy of oxidation lost as heat 
Types of Uncouplers: 
1. Chemical uncouplers – example 2, 4-dinitrophenol (2, 4-DNP) 2, 4, - DNP accepts proton and carries it into matrix through IMM (membrane permeable) 
2. Physiological uncoupler – thermogenin (protein) H+ -channel in the IMM 
Abundant in mitochondria of brown adipose tissue (low level of ATP synthase activity) Responsible for diet induced thermo-genesis Brown adipose tissue is absent or reduced in obese individuals Present in newborns and cold adapted individuals Thermogenin is opened by fatty acids liberated upon degradation of stored fat by activated hormone sensitive lipase by norepinephrine released in response to drop in body temperature due to cold environment. Opening of thermogenin allows reentry of translated protons through IMM (no proton gradient formed No ATP synthesis Energy of oxidation lost as heat biological importance - maintain body temperature in newborns - cold adaptation 

f- Respiratory Poisons 

Inhibit electron flow through respiratory chain 
Inhibit proton translocation 
Inhibit proton gradient formation 
Inhibit O2 consumption 
Inhibit ATP synthesis 
Reducing equivalents remain reduced 
Other aerobic oxidation’s inhibited (Kreb’s cycle, pyruvate oxidation, fatty acid oxidation)