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      Electrochemically Induced Nuclear Fusion of Deuterium


                        Martin Fleischmann
                     Department of Chemistry
                          The University
                   Southhampton, Hants. S09 5NH
                             ENGLAND


                          Stanley Pons*
                     Department of Chemistry
                        University of Utah
                   Salt Lake city, UT 84112 USA


Submitted to Journal of Electroanalytical Chemistry March 11, 
1989; in final form March 20, 1989 

* To whom correspondence should be addressed.




INTRODUCTION

The strange behavior of electrogenerated hydrogen dissolved in 
palladium has been studied for well over 100 years and, latterly 
these studies have been extended to deuterium and tritium [1].  
For discharge of deuterium from alkaline solutions of heavy water 
we have to consider the reaction steps: 


                       -              -
                D O + e   -> D    + OD                        (i)
                 2            ads

                              -           -
                D    + D O + e  -> D  + OD                   (ii)
                 ads    2           2


                D    -> D                                   (iii)
                 ads     lattice



                D    + D    -> D                             (iv)
                 ads    ads     2


It is known that at potentials negative to +50 mV on the 
reversible hydrogen scale the lattice is in the beta-phase, 
hydrogen is in the form of protons (as shown by the migration in 
an electric field) and is highly mobile (D = 10E-7 cm*cm/s for 
the alpha-phase at 300K). 

The overall reaction path of D2 evolution consists of steps (i) 
and (ii) [2] so that the chemical potential of dissolved D+ is 
normally determined by the relative rates of these two steps.  
The establishment of negative overpotentials on the outgoing 
interface of palladium membrane electrodes for hydrogen discharge 
at the ingoing interface [3] (determined by the balance of all the 
steps i) to (iv)) demonstrates that the chemical potential can be 
raised to high values. Our own experiments with palladium 
diffusion tubes indicate that values as high as 0.8 eV can 
readily be achieved [4] (values as high as 2eV may be achievable).  
The astronomical magnitude of this value can readily be 
appreciated; attempts to attain this level via the compression of 
D2 (step (iv)) would require pressures in excess of 10E24 
atmospheres.  In spite of this high compression, D2 is not 
formed; i.e. the s-character of the electron density around the 
nuclei is very low and the electrons form part of the band 
structure of the overall system.  A feature which is of special 
interest and which prompted the present investigation is the very 
high H/D separation factor for absorbed hydrogen and deuterium 
(see Figs. 4 and 6 of Ref [2]).  This can only be explained if 
the H+ and D+ in the lattice behave as classical oscillators 
(possibly as delocalised species) i.e. they must be in very 
shallow potential wells.  In view of the very high compression 
and mobility of the dissolved species there must therefore be a 
significant number of close collisions and one can pose the 
question: would nuclear fusion of D+ such as 


                2    2     3              1
                 D +  D ->  T(1.01 MeV) +  H(3.02 MeV)        (v)
or
                2    2     3
                 D +  D ->  He(0.82 MeV) + n(2.45 MeV)       (vi)


be feasible under these conditions?



EXPERIMENTAL

In the work reported here D+ was compressed galvanostatically 
into sheet, rod and cube samples of Pd from 0.1 M LiOD in 99.5% 
D2O + 0.5% H2O solutions.  Electrode potentials were measured 
with respect to a Pd-D reference electrode charged to the alpha-
beta-phase equilibrium.  We report here experiments of several 
kinds: 

1)      Calorimetric measurements of heat balances at low current 
densities (=1.6 mA/cm*cm) were made using a 2mm x 8cm x 8cm Pd 
sheet cathode surrounded by a large Pt sheet counter electrode. 
Measurements were carried out in Dewar cells maintained in a 
large constant temperature water bath (300K), the temperature 
inside the cell and of the water bath being monitored with 
Beckman thermometers.  The Heavy Water Equivalent of the Dewar 
and contents and the rate of Newton's law of cooling losses were 
determined by addition of hot D2O and by following the cooling 
curves. 


2)      Calorimetric measurements at higher current densities 
were carried out using 1, 2 and 4mm diameter x 10 cm long Pd rods 
surrounded by a Pt wire anode wound on a cage of glass rods.  The 
Dewars were fitted with resistance heaters for the determination 
of Newton's law of cooling losses; temperatures were measured 
using calibrated thermistors.  Experiments with rods up to 2 cm 
in diameter will be reported elsewhere [5].  Stirring in these 
experiments (and in those listed under 1)) was achieved, where 
necessary, by gas sparging using electrolytically generated D2.  
Measurements at the highest current density reported here
(512 mA/cm*cm) were carried out using rods of 1.25 cm length; the 
results given in Table 1 have been rescaled to those for rods of 
10 cm length. 



3) The spectrum of gamma-rays emitted from the water bath due to 
   the (n,gamma) reaction 


                1                   2
                 H + n(2.45 MeV) ->  D + gamma(2.5 MeV)     (vii)



was determined using a sodium iodide crystal scintillation 
detector and a Nuclear Data ND-6 High Energy Spectrum analyzer.  
The spectrum was taken above the water immediately surrounding an 
0.8 x 10 cm Pd-rod cathode charged to equilibrium; it was 
corrected for background by subtracting the spectrum over a sink 
(containing identical shielding materials) 10 m from the water 
bath. 

The neutron flux from a cell containing a 0.4 x 10 cm Pd-rod 
electrode was measured using an Harwell Neutron Dose Equivalent 
Rate Monitor, Type 95/0945-5.  The counting efficiency of this 
Bonner-sphere type instrument for 2.5 MeV neutrons was estimated 
to be  2.4 x 10E-4 and was further reduced by a factor of 100 due 
to the unfavorable configuration (the rod opposite the BF  filled 
                                                         3
detector).  The background count was determined by making 
measurements 50m from the laboratory containing the experiments; 
both locations were in the basement of a new building which is 
overlain by 5 floors of concrete.  In view of the low counting 
efficiency, counting was carried out for 50 hours.  Measurements 
on a 0.4 x 10 cm rod electrode run at 64 mA/(cm*cm) gave a 
neutron count 3 times above that of the background. 


4)      The rate of generation/accumulation of tritium was 
measured using similar cells (test tubes sealed with Parafilm) 
containing 1 mm diameter x 10 cm Pd rod electrodes.  Measurements 
on the D/T separation factor alone were made using an identical 
cell containing a 1 mm diameter x 10 cm Pt electrode (this 
measurement served as a blank as the H/D separation factors on Pd 
and Pt are known to be closely similar).  1 ml samples of the 
electrolyte were withdrawn at 2 day intervals, neutralised with 
potassium hydrogen phthalate and the T-content was determined 
using Ready Gel liquid scintillation "cocktail" and a Beckman LS 
5000 TD counting system.  The counting efficiency was determined 
to be about 45% using standard samples of T-containing solutions.  
The beta-decay scintillation spectrum was determined using the 
counting system. 

In these experiments standard additions of 1 ml of the electrolyte 
were made following sampling.  Losses of D2O due to electrolysis 
in these and all the other experiments recorded here were made up 
using D2O alone.  A record of the volume of D2O additions was 
made for all the experiments. 

In all of the experiments reported here all connections were 
fitted into Kel-F caps and the caps were sealed to the glass 
cells using Parafilm. 

Results for the mass spectroscopy of the evolved gases and full 
experimental details for all the measurements will be given 
elsewhere [5]. 


RESULTS

1) and 2)

In the calorimetric experiments we can set lower and upper bounds 
on the rates of Joule heating depending on whether reactions (i), 
(ii) , and (iv) are balanced by 


                   -                 -
                4OD  -> D O + O  + 4e                      (viii)
                         2     2


at the anode or by the reverse of reactions (i), (ii), and (iv).  
In the former case the Joule heating is simply the cell current 
multiplied by (cell voltage - 1.54 V) where 1.54 V is the cell 
voltage at which reactions (i), (ii), and (iv) balanced by (viii) 
are thermoneutral: irreversibilities in the electrode reactions 
and ohmic resistance losses have identical effects on the Joule 
heating.  However, if reactions (i), (ii), and (iv) are reversed 
at the anode and, equally, if the reverse of reactions (viii) 
contributes to the cathode processes, then we get an upper bound 
to the Joule heating which is simply the cell current multiplied 
by the cell voltage. 

We have confirmed in long duration experiments that the rates of 
addition of D2O to the cells required to maintain constant 
volumes are those for reactions (i), (ii), and (iv) balanced by 
reaction (viii). Furthermore, subtraction of the ohmic potential 
losses in solution for the cell containing the large Pt-anode 
shows that the electrolysis of D2O is the dominant process, i.e. 
we have to assume that the Joule heating is close to the lower 
bound. 

Table 1 gives the results for experiments designed to cover the 
effects of electrolyte geometry, electrode size, current density 
(or overpotential) method of operation, etc.  The nature and 
large magnitude of the effects can be appreciated from the 
following observations: 



a)      excess enthalpy generation is markedly dependent on the 
applied current density (i.e. magnitude of the shift in the 
chemical potential) and is proportional to the volume of the 
electrodes; i.e. we are dealing with a phenomenon in the bulk of 
the Pd-electrodes. 



b)      enthalpy generation can exceed 10 watts/(cm*cm*cm) of the 
palladium electrode; this is maintained for experimental times in 
excess of 120 hours during which typically heat in excess of 
4MJ/(cm*cm*cm) of electrode volume was liberated.  It is 
inconceivable that this could be due to anything but nuclear 
processes. 



c)      in research on thermonuclear fusion, the effects are 
expressed as a percentage of the breakeven where 100% breakeven 
implies that the thermal output equals the input (neglecting the 
power required to drive the equipment).  In electrochemical 
experiments we have additionally to take into account whether 
breakeven should be based on the Joule heat or total energy 
supplied to the cell.  Furthermore, in the latter case the energy 
supplied depends on the nature of the anode reaction.  Table 2 
lists three such figures of merit and it can be seen that we can 
already make reasonable projections to 1000%.  Some of the 
factors important to scale-up are already apparent from Tables 1 
and 2. 



d)      the effects have been determined using D2O alone.  
Projections to the use of appropriate D2O/DTO/T2O mixtures (as is 
commonly done in fusion research) might therefore be expected to 
yield thermal excesses in the range 10E3 - 10E4 % (even in the 
absence of spin polarisation) with enthalpy releases in excess of 
10 kW/(cm*cm*cm).  We have to report here that under the 
conditions of the last experiment even using D2O alone, a 
substantial portion of the cathode fused (melting point 1554 
degrees C) part of it vapourised and the cell and contents and a 
part of the fume cupboard housing the experiment were destroyed. 



TABLE 1. Generation of excess enthalpy in Pd-cathodes as a 
function of current density and electrode size. 

Cube        Sheet      Rod       Rod       Rod        electrode type
                     
1x1x1 cm    0.2x8x8cm  0.4x10cm  0.2x10cm  0.1x10cm   dimensions

125         0.8        8         8         8          current density (mA/cm*cm)

WARNING     0.153      .153      .036      .0075      excess rate of heating
                                                      (watts/cm*cm*cm)
IGNITION?
(see text)  0          .122      .115      .095       excess specific rate of
                                                      heating (watts/cm*cm*cm)

250         1.2        64        64        64         current density (mA/cm*cm)

            .027       1.751     .493      .079       excess rate of heating
                                                      (watt)

            .0021      1.39      1.57      1.01       excess specific rate of
                                                      heating (watts/cm*cm*cm)

            1.6        512       512       512        current density * 
                                                      (mA/cm*cm) *

            0.79       26.8      3.02      .654       excess rate of heading
                                                      (watt) *

            .0061      21.4      9.61      8.33       excess specific rate of
                                                      heating (watts/cm*cm*cm)


 * Measured on electrodes of length 1.25 cm and rescaled to 10 cm.

TABLE 2. Generation of excess enthalpy in Pd rod cathodes 
expressed as a percentage of breakeven values. 

0.4x10cm    0.2x10cm   0.1x10cm   dimensions
8           8          8          current density (mA/cm*cm)
111         62         23         excess heating * (% of breakeven) * 
53          27         12         excess heating** (% of breakeven) **
1224        286        60         excess heating*** (% of breakeven) ***
64          64         64         current density (mA/cm*cm)
66          46         19         excess heating * (% of breakeven) *
45          29         11         excess heating** (% of breakeven) **
438         247        79         excess heating*** (% of breakeven) ***
512         512        512        current density (mA/cm*cm)
59          14         5          excess heating * (% of breakeven) *
48          11         5          excess heating** (% of breakeven) **
839         189        81         excess heating*** (% of breakeven) ***

*       % of breakeven based on Joule heat supplied to 
        cell and anode reaction 

           -                  -
        4OD  -> 2D O + O  + 4e
                  2     2

**      % of breakeven based on total energy supplied to 
        cell and anode reaction 

           -                  -
        4OD  -> 2D O + O  + 4e
                  2     2

***     % of breakeven based on total energy supplied to 
        cell and for an electrode reaction 

                -             -
        D  + 2OD  -> 2D O + 4e 
         2             2

       with a cell potential of 0.5V.

                 2    2
All %'s based on  D +  D reactions, i.e. no projection 
to [next line lost in scanning]


3)      Fig. 1A illustrates the gamma-ray spectra which have been 
recorded in regions above the water bath adjacent to the 
electrolytic cells and this spectrum confirms that 2.45 MeV 
neutrons are indeed generated in the electrodes by reaction (vi).  
These gamma-rays are generated by the reaction (vii).  We note 
that the intensities of the spectra are weak and, in agreement 
with this, the neutron flux calculated from the measurements with 
the dosimeter is of the order 4 x 10E4 1/s for a 0.4 x 10 cm rod 
electrode polarised at 64 mA/(cm*cm). 


Figure 1A

gamma-ray spectrum recorded above the water bath containing the 
rod cathodes.  Measurements carried out with a sodium iodide 
crystal scintillation detector and a Nuclear Data ND-6 High 
Energy Spectrum Analyzer.  The background in this region (taken 
over a water bath 5 m from the experiment containing identical 
shielding materials) is level at about 400 counts; spectrum 
accumulation time: 48 hours. 


4)      In agreement with this low neutron flux, the accumulation 
in the electrolyte also indicates a low rate for reaction (v) 
(which has been found to be somewhat faster than (vi) in high 
energy physics experiments).  The time dependent fraction of 
tritium in the solvent can be shown to follow(?) 


(1):
                        -(1 + lambda * delta   )*Rt
                                            D,T
alpha  =   gamma  * exp ---------------------------
     T          T            lambda * S    * N
                                       D,T


                                                 delta
                                                      D,T
         + ((1 + lambda)gamma  + beta/R) * --------------------- * -+
                             T             (1 + lambda*delta   )    |
                                                            D,T     |
								    |
			+-------------------------------------------+
			|
			|	           -(1 + lambda * delta   )Rt
                        |      				       D,T
			+-->	* (1 - exp --------------------------)
				                lambda*S   * N
				                        D,T

where:

gamma  is the fraction of T in the electrolyte/solvent feeds,
     T

lambda * R (atoms T/s, here 4x10E11 atoms/s) is the sampling rate 
           which has been assumed to be continuous in time,

N is the total number of atoms of D in the Dewar (14.6x10E23),

S    is the D/T separation factor,
 D,T

beta is the rate of the nuclear reaction (v) (events/s), and

R is the rate of electrolysis expressed as atoms D 1/s
  (here 1.24x10E14(?) atoms/s)

It can be seen that the final value alpha  for the cell containing
                                         T
the Pt-cathode (for which we assume beta  = 0) is:
                                        A


                                                delta
                                                     D,T
alpha  = ((1 + lambda)*gamma  + beta/R) * ----------------------   (1)
     T                      T             (1 + lambda * delta   )
                                                             D,T


Blank experiments using Pt-cathodes (which have very similar 
separation factors to Pd) indicate little accumulation of DTO so 
that S    is close to unity under the conditions of our 
      D,T
experiments.  DTO accumulates in the cells containing Pd cathodes 
to the extent of about 100dpm/ml of electrolyte and Fig. 1B 
demonstrates that the species accumulated is indeed tritium.  Use 
of equation (2) then indicates that reaction (v) takes place to 
the extent of 1-2 x 10E4 atoms/s which is consistent with the 
measurements of the neutron flux, bearing in mind the difference 
in radii.  On the other hand the data on enthalpy generation 
would require rates for reactions (v) and (vi) in the range 10E11-
10E14 atoms/s.  It is evident that reactions (v) and (vi) are 
only a small part of the overall reaction scheme and that other 
nuclear processes must be involved. 

(see figure on trailing pages)

Figure 1B

beta-ray disintegration scintillation spectrum measured with a 
Bockman LS5000TD counter-spectrometer. 


DISCUSSION

We realise that the results reported here raise more questions 
than they provide answers and that much further work is required 
on this topic.  The observation of the generation of neutrons and 
of tritium from electrochemically compressed D+ in Pd cathode is 
in itself a very surprising result and, evidently, it is 
necessary to reconsider the quantum mechanics of electrons and 
deuterons in such host lattices.  In particular we must ask: is 
it possible to achieve a fusion rate of 10E-19 1/s for reactions 
(v) and (vi) for clusters of deuterons (presumably located in the 
octahedral lattice positions) at typical energies of 1eV?  
Experiments on isotopically substituted hydrides of well defined 
structures might well answer this question. 

The most surprising feature of our results however, is that 
reactions (v) and (vi) are only a small part of the overall 
reaction scheme and that the bulk of the energy release is due to 
an hitherto unknown nuclear process or processes (presumably 
again due to clusters of deuterons).  We draw attention again to 
the very large magnitude of the effects in the confinement 
parameter diagram, fig. 2.  We note that the values of the 
confinement parameter are extremely high compared to conventional 
research on fusion (high particle densities, lifetimes of 10E2 - 
10E4 years) while the chemical potential is very low compared to 
the equivalent parameter, (T), in those experiments.  It is 
evident that diagrams of this kind require extension in the third 
dimension for electrochemical experiments since the results are 
so markedly dependent on electrode volume (increase of current 
density displaces the points in a vertical direction).  We draw 
attention again to the fact that the experiments already carried 
out are close to the breakeven point; further work to extend the 
electrode dimension (and to establish the nature of the processes 
responsible for the enthalpy release) is in progress. Finally, we 
urge the use of extreme caution in such experiments: a plausible 
interpretation of the experiment using the Pd-cube electrode is 
in terms of ignition.  Projection of the values in Tables 1 and 2 
to more extreme conditions indicate that this may indeed be 
feasible. 

Figure 2

                                                          2    2
Confinement parameter-chemical potential-size diagram for  D +  D 
                                                  2    3
fusion reaction in Pd-cathodes, projection to the  D +  T 
reaction. 


ACKNOWLEDGEMENT

We wish to thank Johnson Matthey PLC for the loan of precious 
metals for this project. 


LITERATURE REFERENCES

1. W. M. Mueller, J. T. Blacklodge, G. G. Libowitz, "Metal 
   Hydrides", Academic Press, New York (1968); G. Bambakadis, Ed., 
   "Metal Hydrides", Plenum Press (1981). 

2. B. Dandapani and M. Fleischmann, Journal of Electroanalytical 
   Chemistry, 12 (1972) 323.2.39

3. A. N. Frumkin and N. A. Aladzhalova, Acta Physicochim.
   U.R.S.S., 2 (1940) 1.9

4. Unpublished results

5. M. Fleischmann, M. Hawkins, and B. Pons, to be published.

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