American Journal of Environmental Protection
Volume 5, Issue 3-1, June 2016, Pages: 21-25

An Approach to Removing Large Quantities of Atmospheric Greenhouse Gases

John B. Cook1, Svetlana R. Amirova2, Edwin A. Roehl Jr.1, Paul A. Comet3, Tamara V. Tulaykova4

1Advanced Data Mining International, Greenville, S.C, USA

2Brody School of Medicine, East Carolina University, Greenville, North Carolina, USA

3Comet Environmental Consulting, Houston, Texas, USA

4Wave Research Center at A. M. Prokhorov’s General Physics Institute, Moscow, Russia

Email address:

(J. B. Cook)
(T. V. Tulaykova)
(Edwin A. R. Jr.)
(P. A. Comet)
(S. R. Amirova)

To cite this article:

John B. Cook, Svetlana R. Amirova, Edwin A. Roehl Jr., Paul A. Comet, Tamara V. Tulaykova. An Approach to Removing Large Quantities of Atmospheric Greenhouse Gases. American Journal of Environmental Protection. Special Issue: New Technologies and Geoengineering Approaches for Climate. Vol. 5, No. 3-1, 2016, pp. 21-25. doi: 10.11648/j.ajep.s.2016050301.14

Received: March 24, 2016; Accepted: March 27, 2016; Published: May 10, 2016

Abstract: A method for removing atmospheric carbon dioxide (СО2) and water vapor is proposed. The method sprays clouds with alkaline compounds to significantly increase the solubility of СО2 in the cloud water, providing for much higher than normal levels of СО2 to be absorbed by rain droplets. The CO2 is transported to the ground for sequestration in surface and/or ground water, and available for carbon fixation by plants and organisms. Presented calculations estimate that 38 gigatonnes of atmospheric CO2 could be removed per year by applying the process over 0.08% to 2.4 % of the Earth’s surface. Laboratory experiments that grew multiple edible plant species irrigated with the modified rainwater indicated yield benefits. A concept for removing atmospheric methane (CH4) is also presented. Powerful lasers would ionize the CH4 to form CO2 that could then be removed by the alkaline-enhanced rainfall method.

Keywords: Climate Change, Greenhouse Gas, Carbon Dioxide, Methane, Water Vapor, Removal, Alkali, pH Adjustment, Precipitation, Cloud Seeding, Laser

1. Introduction

Current global emissions of greenhouse gases are exceeding the Earth’s assimilative capacity, causing them to accumulate in the atmosphere [1], [2]. Water vapor comprises 95% of all greenhouse gases [3], however, carbon dioxide (CO2) and methane (CH4) are of greater concern. Higher greenhouse gas concentrations are widely believed to contribute to climate change, extreme weather events, rising sea levels, and other marked changes, such as the acidification of surface waters and soils.

Over the past century the carbon dioxide (CO2) concentration rose from 280 to 400 parts per million (ppm), the methane (CH4) concentration rose from 0.9 to 1.8 ppm, and both continue to rise rapidly [4], [5]. The oceans’ natural alkalinity allows them to store a large amount of CO2, including more than a quarter of that produced anthropogenic ally. This has increased ocean acidity ~26% from preindustrial levels, which corresponds to a decrease in pH from an average of 8.2 to 8.1, or less. A further decrease of ~0.3 units by 2100 is likely unless CO2 emissions are reduced rapidly. Higher ocean acidity negatively impacts marine ecosystems and the economic benefits they provide [6], [7]. Similarly, rains in industrial regions since the mid-20th century have caused soil deterioration due to higher acidity, with current pH » 3 – 4 [8], reducing alkalinity in the environment.

The development of methods that can efficiently remove greenhouse gases already in the atmosphere would be beneficial. Precipitation enhancement methods, which de facto remove water vapor, have been developed primarily for agriculture, water supply, and reducing air pollution [9], [10]. Typically, aircraft, rockets, or other projectiles are used to disperse hygroscopic or glacial particles to alter cloud microstructure, inducing precipitation [11], [12]. Seeding along a narrow flight path can be sufficient to restructure an entire cloud. Acoustic wave generators have been investigated as an alternative means to inducing precipitation [13], [14].

A new method proposed here expands the purpose of precipitation enhancement to include climate modification through the removal of large amounts of under-cloud CO2. The solubility of СО2 in water is highly sensitive to pH [15], [16], so the first step is to disperse an alkaline compound such as potassium hydroxide (KOH) inside clouds over selected areas to increase the pH of the clouds’ constituent microscopic water droplets to 10 – 11. The alkaline particles should be consistent in size and composition, and dispersed uniformly inside clouds to produce droplets formed by nucleating water vapor which are uniform in size and pH.

The method’s second step is to induce rain, allowing the high pH rain to absorb substantially more CO2 than a normal pH rain or a two-dimensional (2-D) patch of surface water whose specific surface area is less than rain’s three-dimensional (3-D) droplets. The second step would be unnecessary if alkalis having strong hygroscopic properties are used. Once on the ground, the dissolved CO2 is sequestered in surface and/or ground water, and available for carbon fixation by plants and organisms.

Below are calculations that estimate the efficiency of the proposed method for atmospheric СО2 removal, and results from laboratory experiments that grew different crop species irrigated with the modified rainwater. Also described is a concept that uses laser-induced oxidation to convert atmospheric СH4 into СО2 that can then be removed by the alkaline-enhanced rainfall method.

2. Atmospheric CO2 Removal

The typical pH of normal rainwater ranges from 5.6 to a neutral 7.0, at which the concentrations of dissociated ions are relatively small. The insoluble and dissociated portions of the weak acid that remains after attaining the equilibrium of saturation for water by СО2 are described by (1), where H2CO3 is carbonic acid, H+ is hydrogen ion to determine pH, and HCO3- and CO32- are bicarbonate and carbonate ions.

СО2 + H2O = H2CO3

H2CO3 = HCO3- + H+               (1)

HCO3- = CO32- + H+

The equilibrium concentrations of H2CO3, HCO3-, and CO32- at a neutral pH = 7.0 are approximately 0.71, 3.3, and 0.001 milligrams per liter (mg/l), respectively [17]. СО2 solubility increases as pH increases due to an increasing H+ concentration, with HCO3- and CO32- concentrations increasing by one and two orders of magnitude, respectively, for each unit change in pH. The fractions of carbon in the molar masses of H2CO3, HCO3-, and CO32- are 0.1935, 0.1967, and 0.2, respectively, so all fractions are equal to or approximately equal to 0.2.

The mass of carbon MC(pH) in the dissolved CO2 in a rainfall volume equivalent Uw = hwA is estimated from (2), where hw and A are the volume’s height and cross-sectional area. For brevity, the H2CO3, HCO3-, and CO32 concentrations are referred to as C1, C2(pH), and C3(pH).

MC(pH) » Uw{0.2 [C1 + C2(pH) + C3(pH)]}      (2)

The concentration of atmospheric carbon Ca- in an air volume with a height h and a unit (1 m2) cross-section can be estimated from (3), which is derived from (2). The vertical mixing ratio of CO2 is estimated to be constant for altitudes of interest. The fraction of carbon in the molar mass of CO2 is 12/44 = 0.27. For a cloud at an altitude of 1 km, the cloud water pH should be increased from a typical 5.6 to 10.3 for complete CO2 removal (Ca- = 420 ppm).

Ca- » (hw/h)[0.2(C1 + C2(pH) + C3(pH)]/0.27      (3)

The deployment of KOH in a liquid water aerosol is used to illustrate how to estimate the amount of an alkali needed to raise the pH of cloud water to an effective level. The dissociation reaction of KOH in water represented by (4) indicates that the molar concentrations of KOH and OH- are equal.

An alkali facilitates the dissociation of ionic species in water according to the constant Кw = 10-14at 20°C [17]. According to (4) and (5), the KOH mass concentration nKOH needed to raise the pH of the cloud water from 5.6 to 10 is 10-4 mol/l, or 56x10-4 g/l when converted to a molar mass. For an example 1 km3 cloud having a liquid water concentration of 1 g/m3, the mass of KOH to be dispersed would only be 5.6 kg. Note that little of the KOH would be spent within the cloud over a short period prior to rainfall inducement due to the small resident concentration of СО2 molecules (~400 ppm).

KOH = K+ + OH-                    (4)

H+ + OH- = H2O, Кw = [H+] [OH-]             (5)

The volume of water precipitated by a cloud UI is estimated by (6), where I is the rainfall rate, As is the 2-D receiving area on the Earth’ surface, and T is the duration of the rainfall event. The number of spherical droplets N having a radius rd in UI and the droplets’ total surface area Ad are estimated by (7) and (8) respectively.

UI = I AsT                     (6)

N = 3UI / (4prd3)                 (7)

Ad = N´4prd2                  (8)

If given a moderate rainfall characterized by As = 1 km2 = 106 m2, I = 6 mm/h, T = 1 hour, and rd = 0.5 mm, then UI = 6,000 m3, N = 1013, and Ad = 3.6´107m2 = 36´As. Alternatively, the Marshall-Palmer approximation accurately estimates droplet radii spectra for drizzle, rain, or storm events, and can be applied to perform more detailed droplet surface area estimates [18], [19]. The parameters and measurement methods used to characterize precipitation inside clouds and atmosphere volumes are described in [20][22].

Rapid CO2 saturation of droplets is made possible by their small size and slow speeds. The terminal speed of a droplet Vg is estimated by (9) by equating the forces of gravity and air resistance, where ra and rw are the densities of air and water respectively, and g is the acceleration due to gravity. A droplet having rd = 0.5 mm falling from an altitude h = 1 km has a Vg = 2.9 m/sec (ra = 1.2 kg/m3 at 12°C). The travel time th = 350 seconds is estimated by (10).

Vg = (2rdgrw / ra)½                  (9)

th = h / Vg                      (10)

The time taw needed for a droplet to become saturated with CO2 depends on the ratio of the droplet’s aerated volume to its surface area, and is estimated by (11), where kaw is a measured constant, called the gas transfer velocity, for air and water [23]–[26]. For kaw » 0.5´10-4 m/sec and rd = 0.5 mm, taw = 6 seconds, indicating that the much longer travel time th » 350 seconds is sufficient for nearly complete removal of under-cloud CO2 molecules.

taw = rd / 3kaw                    (11)

2.1. Impact on Plants



Fig. 1. First crop plants after 19 days (a) and 31 days (b) days. The blue pot (left) was irrigated daily with distilled water. The brown pot (right) was irrigated with an alkaline solution.

A potential benefit to plant growth is illustrated by results from indoor bench-scale experiments [27] in which two simulated crops were irrigated with and without alkaline-enhanced water for a period of one month (Figs. 1 and 2). The blue pots were irrigated daily with distilled water, and the brown pots were irrigated using the same regime with a stable KOH-distilled water solution having a pH=12. For the first crop both pots were identically planted with beetroots (10 grains), carrots (20 grains), and parsley (2 grams). For the second crop the pots were planted with dill (20 grains) and cucumber (5 grains). As shown, both crops responded favorably to the alkaline-enhanceme irrigation.

Fig. 2. Second crop plants after 19 days.

2.2. Global Application

Table 1. Estimated Outcomes of Global Application.

pH 5.6 10 10.5 11
MC1 (kg/m2) 1.6´10-4 0.849 4.05 26.5
MAС (kg) 8.2´1010 4.3´1014 2.1´1015 1.4´1016
MAСО2 (kg) 3´1011 1.6´1015 7.7´1015 5´1016
Ap (%) - 2.4 0.5 0.08
QKOH (kg) - 6.9´1010 4.8´1010 2.3´1010

pH = pH of induced rainfall, MC1 = mass of atmospheric carbon removed by 1 meter of rainfall per m2of the Earth’s surface, MAC = mass of global atmospheric carbon removed, MAС02 = mass of global CO2 removed, Ap = percentage of the Earth’s surface area needed to completely remove annual global CO2 emissions (EA), and QKOH = mass of KOH needed to remove EA each year.

Table 1 provides statistics that estimate outcomes of applying the method globally. The Earth’s surface area AE = 5.1´108 km2, the average global annual rainfall hA = 1 m [28], and the annual global CO2 emissions EA » 3.8´1013 kg [29]. Using (2), row 2 gives the masses of atmospheric carbon MC1 removed by 1 meter of annual rainfall per m2of the Earth’s surface at the different pH levels shown in row 1. Row 3 gives the global masses of carbon removed MAC per (12). Row 4 gives the global masses of CO2 removed MAС02 per (13), 0.27 being the carbon ratio of CO2. Using (14), row 5 gives the percentages Ap of AE needed to completely remove annual emissions EA, indicating the need is 0.08% 2.4%. Row 6 gives the mass QKOH of KOH needed to remove EA each year per (15), indicating that the amount needed is a fraction of the 19´1010 kg of nitrogen, phosphorous, and potassium (N/P/K) fertilizers used globally in 2014 [30].

MAC = MC1 AE                  (12)

MAС02 = MAC / 0.27               (13)

Ap = 100 ´ EA/MAС02              (14)

QKOH= nKOH hA AE Ap             (15)

3. Atmospheric CH4 Removal

A concept is also proposed that would use lasers to enhance the conversion of atmospheric CH4 into CO2 and water, a process that occurs naturally through the photo-dissociation of CH4 molecules by sunlight [31]. Once freed, the carbon ions bond preferentially with oxygen [32]. This process can be stimulated by using a powerful laser with an optimized wavelength. Subsequent alkaline-enhanced rainfall would remove the CO2.

Measurements of atmospheric CH4 concentrations can be performed at distances of 8 - 11 km using pulsed integrated-path differential absorption Lidar in the infrared spectrum at wavelengths l = 1,650 nanometers (nm) [33], [34]; however, the photon energies are too low for ionization. For efficient ionization, the laser wavelength should coincide with a peak absorption frequency at the molecule’s C-H bond dissociation energy of E » 4.3 eV electronvolts (eV) or l = 288 nm due to the Planck–Einstein relation λE = hc = 1240 eVnm, where h is the Planck constant and c is the speed of light [35]. However, at UV irradiation other gases such as oxygen and nitrogen also could be ionized. Alternatively, multiple-photon excitation achieves photo-dissociation using a laser to bombard gas molecules with multiple photons, increasing their vibrational energy until their chemical bonds are broken [36]. CH4 has a small absorption peak near l = 865 nm (1.43 eV) [37], suggesting that three or four photons could be sufficient for dissociation to occur.

4. Conclusions

A proposed approach could be effective at removing significant amounts of the main greenhouse gases of concern, i.e., water vapor, CO2, and CH4. Estimates show that a method for alkaline-enhanced rainfall could remove more than the ~38 gigatonnes of anthropogenic CO2 emitted each year if applied over a small portion of Earth’s surface. The next step would be to field test the method’s efficacy. An adjunct method for pre-treating atmospheric CH4 by laser is also proposed. It would convert the CH4 into CO2 for subsequent removal by alkaline-enhanced rainfall.


The authors thank Dr. Yakov Ponurovskii and Dr. Imant Vinorgadov for sharing information about monitoring greenhouse gases with tunable diode laser spectroscopy and the photo-dissociation of methane with lasers.


  1. IPCC, Contribution of Working Group III to the Fifth Assessment Report of the Intergovernmental Panel on Climate Change. Summary for Policymakers, Cambridge University Press, New York, 2014.
  2. Kleidon, A., Malhi, Y. and Cox, P. M., "Maximum entropy production in environmental and ecological systems introduction," Philos. Trans. R. Soc. B 365, 1297-1302. 2010.
  3. Freidenreich, S.M. and Ramaswamy, V., "Solar radiation absorption by carbon dioxide, overlap with water, and a parameterization for general circulation models," J. of Geophys. Res. 98, 7255-7264. 1993.
  4. Latest reading, Mauna Loa Observatory. 2016. [Accessed Apr. 4, 2016].
  5. Schmidt, G., "Methane: a scientific journey from obscurity to climate super-stardom," NASA Goddard Space Center, 2004.[Accessed Apr. 4, 2016].
  6. Andersson, A. J. and Gledhill, D., "Ocean acidification and coral reefs: effects on breakdown, dissolution, and net ecosystem calcification," Annu Rev Mar Sci 5, 1.1–1.28, 2013.
  7. Secretariat of the Convention on Biological Diversity, Roberts, J.M. and Williamson, P. – ed., An Updated Synthesis of the Impacts of Ocean Acidification on Marine Biodiversity, Technical Series No. 75, Montreal, Canada, 2014.
  8. Izrael, Y.A. et al., Acid rain (Hydrometeoisdat,Russia, 1989).
  9. Langmuir, I., "Improved methods of conditioning surfaces for adsorption" J. Am. Chem. Soc. 59. 1762-1763. 1937.
  10. Dennis, A.S., Weather modification by cloud seeding, Academic Press, New York, 1980.
  11. Shmeter, S.M. and Berynlev, G.P., "Efficiency of cloud and precipitation modification with hygroscopic aerosols," Meteorology and Hydrology Rus., 2. 43-60. 2005.
  12. Tulaikova, T., Mihtchenko, A. and Amirova, S., "Micro physical model for glaciogenic particles in clouds for precipitation enhancement," Am. J. Env. Protection, 5(3-1). 10-14. 2016.
  13. Tulaikova, T. et al., Acoustic rains, Physmathbook, Moscow, 2010.
  14. Claus R.O. and Tulaikova, T.V., "New methods for helicopter for free flight inside clouds and precipitation enhancement," Am. J. Env. Protection, 5. 1-9. 2016.
  15. Yunge, H., Chemical compounds and radio-activity in the atmosphere, Clarendon, Oxford, 1965.
  16. Rasool, S. I. (ed.), Chemistry of the lower atmosphere, Plenum, New York, 1973.
  17. Sillen, L.G. (ed.), Stability constants of metal-ion complexes, Chemical Society, London, 1964.
  18. Borovikov, A.M., Physics of clouds, Hydromet-Press, Leningrad, Russia, 1961.
  19. Kobayashi, S.T. et al, "Backscattering enhancement on spheroid-shaped hydrometeors: considerations in water and ice particles of uniform size and Marshall-Palmer distributed rains," Radio Science, 42. Apr.2007.
  20. Bruintjes, R.T., "A review of cloud seedingexperiments to enhance precipitation and some new prospects," BAMS, 90. 805-820. 1999.
  21. Daly, C. et al, "Observation bias in daily precipitation measurements at United States cooperative network stations," BAMS 88. 899-912. 2007.
  22. Taylor, J.W. et al, "Aerosol measurements during COPE: composition, size and sources of CCN and IN at the interface between marine and terrestrial influences," Atmos. Chem. Phys. Discuss., doi:10.5194/acp-2016-84, in review. 2016.
  23. Hoover, T.E., "CO2 exchange at the air-sea interface," J. Geoph.Res 74. 456-464. 1969.
  24. Liss, P.S., "Processes of gas exchange analysis an air-water interface," Deep-Sea Res. 20. 221-238. 1973.
  25. Broecher, H.C., "The influence of wind on CO2 exchange in a wind-water tunnel including the effect of minelayers," J.Mar. Res. 36. 595-610. 1978.
  26. Wanninkhof, R., "Chemical enhancement of CO2 exchange in natural water," Limnol. Oceanogr., 41. 689-687. 1996.
  27. Tulaikova, T., and Amirova, S.,"The method for effective CO2 purification in the atmosphere," Global J. Sc. Frontier Res., 15-H (1).1-9. 2015.
  28. Rees, G. and Rees, W., Physical principles of remote sensing, Cambridge University Press, 2013, 125.
  29. Olivier, J., Janssens-Maenhout, G., Muntean, M. and Peters, J., Trends in global CO2 emissions: 2015 report,PBL Netherlands Environmental Assessment Agency, 2015.
  30. Food and Agriculture Organization of the United Nations, "World fertilizer trends and outlook to 2018," Rome, Italy, 2015.
  31. Sheu, J., Mokheimer, E. and Ghoniem, A., "A review of solar methane reforming systems,"Int. J. Hydrogen Energy, 40. 12929-12955. 2015.
  32. Clark, J.,Calculations in AS/A Level Chemistry,Pearson Education, London, 2000.
  33. Dawsey, M. et al, "Optical parametric technology for methane measurements," Proc. 2015 SPIE, Lidar Remote Sensing for Environmental Monitoring XV, San Diego, USA.
  34. Riris, H. et al, "Airborne measurements of atmospheric methane column abundance using a pulsed integrated-path differential absorption Lidar,"Applied Optics, 51 (34). 8296- 8305. 2012.
  35. Schmidt, W., Optical spectroscopy in chemistry and life sciences, Wiley-VCH, Germany, 2005.
  36. Cantrell, C.D. (ed.), Multiple-photon excitation and dissociation of polyatomic molecules, Springer, New York, 1986.
  37. Brien, J. and Cao, H., "Absorptionspectra and absorption coefficients for methane in the 750–940 nm region obtained by intracavity laser spectroscopy,"J. Quant. Spec. Rad. Tran., 75 (3). 323-350. Oct.2002.

Article Tools
Follow on us
Science Publishing Group
NEW YORK, NY 10018
Tel: (001)347-688-8931