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Mercury(I) Chloride in Vivo Oxidation: a Thermodynamic Study

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Mercury(I) Chloride in Vivo Oxidation: a Thermodynamic Study Main Group Met. Chem. 2015; 38(3-4): 121–124 Short Communication Aliyar Mousavi* Mercury(I) chloride in vivo oxidation: a thermodynamic study DOI 10.1515/mgmc-2015-0012 of immortality; however, his death in middle age and his Received April 2, 2015; accepted May 19, 2015; previously published slow bodily decay together suggest that he might have died online June 13, 2015 because of ingesting too much Hg (Wright, 2001). In the article ‘Mercury Speciation and Safety Evalu- Abstract: Mercury (Hg) has a long history of both medici- ation of Cinnabar-Containing Traditional Medicines: A nal uses and toxic effects. Hg chlorides were used as med- Mini-Review’, Beers and Mousavi (2013) state that when icines; however, ‘corrosive sublimate’ (HgCl2) was also there was an outbreak of syphilis in Europe at the end of used as a violent poison in the Middle Ages. In this work, the 15th century, ointments and pills of mercury(I) chlo- certain thermodynamic principles of reactivity were used ride (Hg2Cl2), commonly named ‘calomel’, and mercury(II) to show that ingested aqueous calomel (Hg2Cl2) in the chloride (HgCl2) were used for the treatment. They also human stomach is almost entirely converted to HgCl2. This refer to the fact that HgCl2, called ‘corrosive sublimate’, work opens the way to a new series of studies on poison- was used as an antiseptic. In fact, several medicinal uses ing cases in history. (both external and internal) of Hg2Cl2 and HgCl2 are listed in Merck’s 1907 Index (1907). Still, HgCl2 is a violent poison Keywords: calomel; corrosive sublimate; mercury; that had a wide use as such in the Middle Ages ( Greenwood Napoleon. and Earnshaw, 1994), and Merck’s 1907 Index (1907) men- tions ‘corrosive mercury chloride’ as one of its names. In studying poisoning cases in historical perspective, it is therefore important to ask if ingested aqueous Hg Cl in Alchemists regarded mercury (Hg) as a key to the trans- 2 2 the human body is converted to HgCl to any toxicologi- mutation of base metals to gold for over a 1000 years, up 2 cally relevant degree. Such experiments are complicated to 1500 AD (Greenwood and Earnshaw, 1994), and both by the expenses and the toxic effects of Hg. In this article, elemental Hg and some of Hg compounds have a long thermodynamic principles of reactivity are employed to history of being used medicinally. For example, medieval test the hypothesis that ingested aqueous Hg Cl in the Arabs used elemental Hg in order to treat skin diseases, 2 2 human stomach is significantly converted to HgCl . and the use of mineral cinnabar, which is mainly ( ≥ 96%) 2 When ingested, aqueous Hg Cl is, in the human mercury(II) sulfide (HgS), in traditional Chinese medicines 2 2 stomach, in the presence of hydrochloric acid and air. In and Indian Ayurvedic medicines has 2000 years of history this both acidic and oxidizing environment, the following (Beers and Mousavi, 2013). A relevant case is that of one oxidation-reduction (redox) reaction may be proposed: of the most well-known rulers in Russian history, Ivan the Terrible. On examining Ivan’s remains, it was observed 2 Hg22Cl ()aq ++4 HClO()aq 22()ga→+4 HgCl ()ql2 HO2 ( ) that his bones contained a large amount of Hg, which indi- (1) cated that Hg had been heavily used to treat Ivan for illness Certain thermodynamic principles of reactivity and equa- (Pavlov and Perrie, 2003). However, Hg has a history of tions are used as theoretical methods in order to deter- toxic effects, which is also a long history (Greenwood mine the extent to which ingested aqueous Hg Cl in the and Earnshaw, 1994). For example, the emperor Qin Shi- 2 2 human stomach is converted to HgCl . In other words, huang, who unified China under his rule in 221 BC, seems 2 these methods are employed to determine the value of the to have hit upon Hg as a possible candidate for an elixir equilibrium constant for Eq. (1) at the normal human body ° *Corresponding author: Aliyar Mousavi, Science and Engineering temperature (37 C). Technology Department, Nashua Community College, 505 Amherst The net ionic equation for the proposed reaction is the Street, Nashua, NH 03063, USA, e-mail: [email protected] following: 122 A. Mousavi: Mercury(I) chloride in vivo oxidation 2 Hg 22++()aq ++4 HO()aq ( ga)(→+4 Hg + ql)(2 HO ) o2+ 22 2 (2) H∆ f2 for Hg ()aq =172 kJ /mol, ∆ o + = The employed methods consist of the stepwise calcula- Hf for H0()aq kJ/mol, o tion of the following for the reaction shown by Eq. (2): ∆Hf2 for O0()g = kJ/mol, 1. Standard cell potential (Eo ) o2+ cell ∆Hf for Hg ()aq =171 kJ/mol, and 2. The equilibrium constant (Keq) at 298 K o ∆Hf2 for HO()l =-285.840 kJ/mol. 3. The equilibrium constant (Keq) at 37°C (the normal H∆ o =×[(4 mol 171 kJ /mol) human body temperature) reaction +×((2 mol-285.840 k/J mol-))][()2 mol1× 72 kJ/mol The two half-reactions of the proposed redox reaction are +×()4 mol0 kJ/mol1+×() mol 0 kJ /mol ] =-231.68 kJ as follows: ( per mole of reaction). 22++- Oxidation Hg2 ()aq →+2 Hg ()aq 2 e (3) The equilibrium constant at 37°C (the normal human Reduction 4 HO+ ()aq ++()gl4 e2- → H O() 22 (4) body temperature) can be calculated using Eq. (6), where K = K = 9.4 × 1020, ∆H-o = 231.68 kJ /mol reaction, The standard electrode (half-cell) potentials eq1 eq reaction R = 8.314 J/mol reaction.K, T = (37+273.15) K = 310 K, and (Eo) at 298 K for the oxidation and reduction half- 2 T = 298 K. Solving for K , we have K = K = 2.4 × 1019. This reactions are +0.92 V and +1.23 V, respectively 1 eq2 eq2 eq equilibrium constant, which is at 37°C, is so large that we ( Silberberg and Amateis, 2015), which means that may, in the words of Silberberg and Amateis (2015), say EEoo==-E o ++1.23 V-(0.92 V)=+0.31 V0> . This cell cathodeanode that the proposed reaction ‘goes to completion’ at the shows that the proposed reaction is spontaneous at normal human body temperature. 298 K when all the components are in their standard Although the presence of air in the human stomach states. The calculated standard cell potential here is makes it an oxidizing environment, the reaction shown by only used for calculating the equilibrium constant at the following equation [Eq. (7)] may also [in addition to 298 K, and it is noteworthy that the real cell potential the reaction shown by Eq. (1)] be proposed for ingested (E ) varies with variations in the reaction quotient, cell aqueous Hg Cl . Q, which varies with variations in the concentrations 2 2 of the reactants and the products. Even with a known Hg22Cl ()aq +→2 HCl2()aq HgCl22()aq +H ()g (7) and unchanging concentration of H+(aq) in the human The net ionic equation for this other reaction is the stomach and known and unchanging concentrations 2+ following: of Hg2 (aq) and dissolved O2 (the solubility values of ° 22++ + Hg2Cl2 and O2 at 37 C, respectively), the concentration of Hg22()aq +→2 H2()aq H(g)aq +H)( g (8) Hg2+(aq), which is produced in Eq. (2), at any moment of interest is needed to calculate the reaction quotient for The two half-reactions of this redox reaction are as follows: that moment. It is also worth noting that at the equilib- 22++- Oxidation Hg2 ()aq →+2 Hg ()aq 2 e (9) rium state, Ecell is 0. The equilibrium constant at 298 K can be calculated + - Reduction 2 H(aq))+→2 e H2 ( g (10) using Eq. (5). The standard electrode (half-cell) potentials ERo =( T/nF ) ln K (5) cell eq (Eo) at 298 K for the oxidation and reduction half- reactions are +0.92 V and 0.00 V, respectively According to Eq. (2), n = 4 mol e-/mol reaction. Using ( Silberberg and Amateis, 2015), which means that E0o =+ .31 V, R = 8.314 J/mol reaction.K, T = 298 K, and cell EEoo==-E o 0.00 V-(0+=.92 V) -0.92 V0< . This F = 96485 C/mol e-, we have K = 9.4 × 1020. cell cathodeanode eq shows that this other reaction is nonspontaneous at 298 K In order to calculate the equilibrium constant at 37°C when all the components are in their standard states. (the normal human body temperature), the van’t Hoff The equilibrium constant at 298 K can be calculated equation is used. using Eq. (5). According to Eq. (8), n = 2 mol e-/mol reac- o o = = ln()K/eq2eKHq1 =(-∆ reaction /R)( 1/T21-1/T ) (6) tion. Using E-cell 0.92 V, R 8.314 J/mol reaction.K, - -32 T = 298 K, and F = 96485 C/mol e , we have Keq = 7.6 × 10 . o The ∆H f values (at 298 K) for the reactants and products In order to calculate the equilibrium constant at 37°C in Eq. (2) are as follows (Silberberg and Amateis, 2015): (the normal human body temperature), the van’t Hoff A. Mousavi: Mercury(I) chloride in vivo oxidation 123 o equation [Eq. (6)] is used. The ∆H f values (at 298 K) The Ksp at 37°C (the normal human body temperature) -18 for the reactants and products in Eq. (8) are as follows can be calculated using Eq. (6), where Keq1 = Ksp1 = 1.5 × 10 , o ( Silberberg and Amateis, 2015): ∆H1reaction = 01.98 kJ /mol reaction, R = 8.314 J/mol reac- = = = o2+ tion.K, T2 (37+273.15) K 310 K, and T1 298 K.
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