Future Energy Paints as a Scalable and Effective Radiative Cooling Technology for Buildings

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Future Energy Paints as a Scalable and Effective Radiative Cooling Technology for Buildings
Please cite this article in press as: Mandal et al., Paints as a Scalable and Effective Radiative Cooling Technology for Buildings, Joule (2020),
 https://doi.org/10.1016/j.joule.2020.04.010

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Future Energy
Paints as a Scalable                              co-founder and chief scientific officer            to outer space, so the surface sponta-
                                                  of SkyCool Systems, a startup commer-              neously cools, even under strong sun-
and Effective                                     cializing radiative cooling technolo-              light. The passive operation and net
Radiative                                         gies. Dr. Raman’s research interests               cooling effect overcome the disadvan-
                                                  include nanophotonics, metamaterials,              tages of active cooling methods. Since
Cooling Technology                                radiative heat transfer, and energy ap-            the surfaces of buildings exchange
for Buildings                                     plications, including radiative cooling.           large amounts of heat with their envi-
                                                  His works have been published in lead-             ronment as radiation, this makes
Jyotirmoy Mandal,1,*
                                                  ing journals such as Nature, Nature                PDRC attractive for cooling buildings.
Yuan Yang,2 Nanfang Yu,2
                                                  Energy, Physical Review Letters, and
and Aaswath P. Raman1,*
                                                  Joule.                                             Research on radiative cooling has a
                                                                                                     rich history, with materials like poly-
Jyotirmoy Mandal completed his PhD
                                                                                                     mers (e.g., poly(4-methyl-1-pentene)
in Applied Physics at Columbia Univer-            Introduction
                                                                                                     and poly(vinyl fluoride)), dielectrics
sity in the City of New York and is               As climate change and global energy
                                                                                                     (e.g., SiOX, ZnSe), polymer compos-
currently a Schmidt Science Fellow                consumption manifest in rising global
                                                                                                     ites, and paints investigated for their
and a postdoctoral researcher at Uni-             temperatures and heat-islands, cool-
                                                                                                     cooling properties since the 1960s.2,3
versity of California, Los Angeles. His           ing living environments has become
                                                                                                     In the last decade, the field has seen
research interests include low-cost op-           an urgent challenge. In developed set-
                                                                                                     a revival, with reported enhancements
tical designs for radiative cooling and           tings, air conditioning of buildings
                                                                                                     of earlier designs,4–6 and new pho-
solar heating, with a focus on applica-           consumes energy, generates heat,
                                                                                                     tonic7 and polymeric1 ones. While
tions in developing countries.                    and releases greenhouse gases, exac-
                                                                                                     these are efficient at cooling, their util-
                                                  erbating cooling needs. In regions of
                                                                                                     ity depends on the application. For
Yuan Yang is an associate professor in            the world such as South Asia and
                                                                                                     instance, photonic multilayer films,
the Department of Applied Physics                 sub-Saharan Africa, inadequate power
                                                                                                     which can be tailored to have a high
and Applied Mathematics at Columbia               infrastructure for cooling buildings
                                                                                                     Rsolar and selective єLWIR, attain deep
University in the City of New York. His           has led to rising casualties during sum-
                                                                                                     sub-ambient temperatures useful for
research interests include electrochem-           mers. Passive cooling technologies,
                                                                                                     water-cooled HVAC systems, refrigera-
ical energy storage and thermal energy            which are sustainable alternatives or
                                                                                                     tors, and thermoelectric devices.7,8
management. Dr. Yang has published                complements       to   active     cooling
                                                                                                     While these emerging applications
over 70 peer-reviewed journal articles,           methods, can address these issues.
                                                                                                     hold promise, cooling buildings re-
including in leading journals such as             Here, we consider passive daytime
                                                                                                     mains the largest application of radia-
Science, Proceedings of the National              radiative cooling of building envelopes
                                                                                                     tive    cooling    technologies.      And
Academy of Sciences, Advanced Mate-               and propose that white paints, which
                                                                                                     although photonic designs have made
rials, and Joule.                                 are well adapted for application on
                                                                                                     strides in the area,7 white ‘‘cool-roof’’
                                                  buildings and moderately good at
                                                                                                     paints and materials, which have a
Nanfang Yu is an associate professor              radiative cooling, could be developed
                                                                                                     modest Rsolar (0.8) and high єLWIR
in the Department of Applied Physics              into highly efficient radiative coolers
                                                                                                     (0.95), are currently the most widely
and Applied Mathematics at Columbia               for buildings on a global scale.
                                                                                                     used cooling approach for building en-
University in the City of New York. His
                                                                                                     velopes. Given their inherent scalabil-
research interests include mid-infrared           Passive Daytime Radiative Cooling
                                                                                                     ity, with enhancements in Rsolar, paints
and far-infrared optics, metamaterials,           Passive daytime radiative cooling
                                                                                                     thus have the potential to become an
biophotonics, and biologically inspired           (PDRC) involves the reflection of sun-
                                                                                                     optimal solution for the radiative cool-
flat optics. Dr. Yu’s research has been           light (wavelengths l  0.3–2.5 mm)
                                                                                                     ing of buildings.
published in leading journals like                and radiation of long-wave infrared
Science, Nature Materials, Nature Nano-           (LWIR, l  8–13 mm) heat through the
technology, and Joule.                            respective atmospheric transmission                Radiative Cooling Requirements
                                                  windows into outer space (Figure 1A).              While reflective coatings on buildings
Aaswath P. Raman is an assistant                  When a surface under the sky has a suf-            are known to reduce solar heating,
professor of Materials Science and En-            ficiently high solar reflectance (Rsolar)          PDRC technologies go further to
gineering at the University of Califor-           and LWIR emittance (єLWIR),1 solar heat-           achieve heat loss even under sunlight,
nia, Los Angeles (UCLA). He is also               ing is outweighed by radiative heat loss           potentially doubling the cooling energy

                                                                                                Joule 4, 1–7, July 15, 2020 ª 2020 Elsevier Inc.     1
Future Energy Paints as a Scalable and Effective Radiative Cooling Technology for Buildings
Please cite this article in press as: Mandal et al., Paints as a Scalable and Effective Radiative Cooling Technology for Buildings, Joule (2020),
    https://doi.org/10.1016/j.joule.2020.04.010

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Figure 1. Radiative Cooling by a White Paint
(A) Schematic showing passive daytime radiative cooling by solar reflection and LWIR thermal emission through the atmospheric transmission windows.
Corresponding solar and thermal spectra are shown below.
(B) Schematic showing how high solar reflectance and thermal emittance enable PDRC. It should be noted that at near-ambient temperatures, radiative
transfer ( = radiated heat from emitter – downwelling heat from sky) is small outside the LWIR window, making broadband and selective LWIR emitters
similarly effective at cooling.
(C) Schematic showing cooling powers ( = thermal emission – solar absorption) 1 of emissive coatings (єLWIR  0.95) as a function of R solar (or solar
reflectance index [SRI], which varies linearly with R solar ). R solar > 0.95 usually yields sub-ambient radiative cooling.

2       Joule 4, 1–7, July 15, 2020
Future Energy Paints as a Scalable and Effective Radiative Cooling Technology for Buildings
Please cite this article in press as: Mandal et al., Paints as a Scalable and Effective Radiative Cooling Technology for Buildings, Joule (2020),
 https://doi.org/10.1016/j.joule.2020.04.010

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savings in buildings.9 From a physical            ings, paints readily fulfil these practical        stricts Rsolar to
Please cite this article in press as: Mandal et al., Paints as a Scalable and Effective Radiative Cooling Technology for Buildings, Joule (2020),
    https://doi.org/10.1016/j.joule.2020.04.010

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Figure 2. Optical Properties of Paints and Other Radiative Coolers
(A) Measured spectral reflectances of paints based on TiO2, Al 2 O3 , BaSO 4 , porous P(VdF-HFP) and PTFE, and silvered plastics (from top left to bottom
right). The paint films are all 1 mm thick.
(B) R solar of paints and silvered plastics. APOC 256X paint is rated by the Cool Roof Rating Council as the most reflective on the market. The dotted lines
show the reflectances of TiO 2 powder, spectralon (porous PTFE), and silver and represent the likely upper limits of R solar of TiO 2 -based, polymer-based,
and silvered radiative coolers, respectively. Note that the reflectances were weighted using ASTM G-173 solar spectrum, which assumes a solar zenith
angle of 48.19  . During summertime or in the tropics, the noon-time zenith angle is smaller. Consequently, UV light is stronger and further lowers R solar
of TiO 2 and silver-based designs.
(C) є LWIR of common building materials, paints, and silvered emitters.

In that case, the emittance є arises solely          fewer C-H or O-H bonds, which absorb                  paint. Lastly, because fluoropolymers
from the porous polymer itself.                      sunlight at l  1.2, 1.4, 1.7, and 2.3 mm,            have lower refractive indices (1.38–
                                                     and more C-F bonds, which weakly                      1.43) than acrylics (1.495), they
The second is achievable by using fluo-              absorb at 2.1 mm. Moreover, fluoro-                  enhance scattering by pigments and,
ropolymers such as P(VdF-HFP) or                     polymers absorb less UV than acrylic,                 consequently, Rsolar.
commercially available aqueous P(VdF)                further enhancing Rsolar. The absorp-
variants. Compared to acrylic or sili-               tance can be further lowered by                       The above alterations are compatible
cone, fluoropolymer variants have                    reducing the amount of polymer in the                 with paint design and can significantly

4       Joule 4, 1–7, July 15, 2020
Please cite this article in press as: Mandal et al., Paints as a Scalable and Effective Radiative Cooling Technology for Buildings, Joule (2020),
 https://doi.org/10.1016/j.joule.2020.04.010

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improve Rsolar. Figures 2A and 2B show            highly viable platform for the radiative               Characterizing the weathering and
the results relative to reflectances of           cooling of buildings at large scales.                  failure modes of paints with such mod-
TiO2-based white paints, a super-white                                                                   ifications will be essential for adoption
PTFE-based       reflectance   standard           Challenges and Opportunities                           by the construction industry.
(Spectralon SRM-99), and silvered emit-           While paints hold the potential to
ters. Evidently, in the absence of                achieve optimal optical parameters for                 (3) Reducing glare. While reflection
intrinsic UV absorption, scattering by            radiatively cooling building envelopes,                off white paints is diffuse and less
pigments results in high UV-blue reflec-          challenges and questions remain. The                   intense than those off silvered de-
tance. Reducing polymer content yields            major technical ones in our view are                   signs, it may harm eyesight and
similar results in the NIR wavelengths.           listed below, with potential solutions                 heat dark structures in view. Coating
For the BaSO4 and porous P(VdF-HFP)               (Figure 3).                                            super-white paints with commercial
paint coatings, Rsolar reaches 0.98,                                                                    high-index (n  1.9) retroreflective
and for the Al2O3 and the PTFE-based                  (1) Maximizing Rsolar and єLWIR with               spheres may address the issue.
paint coatings, it exceeds 0.94. These                minimal use of material. Cost re-                  However, their impact on Rsolar and
reflectance values match or even                      mains a central challenge for any                  єLWIR remains unexplored.
exceed those of previously reported                   radiative    cooling     technology,
radiative coolers and, along with the                 including paints, where higher mate-               (4) Color as an aesthetic requirement
high, broadband є (Figure 2C), puts                   rial costs could potentially be a                  and solution to glare. The industry
paints on par with state-of-the-art                   roadblock. To mitigate this, and                   has used selectively visible-absorp-
PDRC designs.                                         reduce material usage, we note                     tive colorants to create NIR-reflective
                                                      that high єLWIR could be achieved                  paints. Recent innovations like fluo-
                                                      by intrinsically emissive pigments                 rescent pigments that convert visible
Complementing PDRC: Paints as a
                                                      with specific microscale sizes, or                 absorption to NIR emission,11 and
Mature Technology
The high PDRC potential of white paints               coating paints on emissive sub-                    the bilayer design discussed above,
is complemented by their generally low                strates. A high Rsolar could be                    where a selectively visible absorbing
cost and ease of application on a broad               achieved by incorporating air voids                colorant is painted atop a broadband
range of surfaces. Furthermore, PDRC                  (n  1) in paints to increase optical              solar scattering layer, could be used
applications of paints can leverage ad-               scattering. Another possibility is                 to maximize the cooling performance
vancements made by the coatings in-                   bilayer designs that exploit the shal-             while achieving color.
dustry in chemical engineering for                    lower penetration by shorter solar
higher durability. Examples include                   wavelengths in paint coatings (Fig-                (5) In view of large-scale applica-
coatings based on silicone, fluoropoly-               ure 3). A thin layer of UV-reflective              tions, reducing the environmental
mer, and cross-linkable binders that                  paint (Figure 2A) could be coated                  impact of paints. Currently, paints
are resistant to UV damage and weath-                 on a TiO2 paint film, affording the                often use environmentally hazard-
ering and remain stable under the sky                 high scattering efficiency of TiO2                 ous pigments that eventually ‘‘run
for years.                                            pigments while reflecting UV light                 off’’ into the environment or, for
                                                      from the top.                                      porous polymeric paints, may use
Due to their long-standing usage,                                                                        toxic solvents like acetone.1 Substi-
paints also have a significant advantage              (2) Durability and resistance to soiling.          tution of such materials with eco-
of being a part of buildings-related en-              Many conventional white paints, while              friendly ones (e.g., water-based flu-
ergy policies worldwide. In the U.S., cit-            engineered for durability, experience              oropolymer variants), as well as
ies like New York and states like Califor-            drops in solar reflectance over time.              enhancing the durability of paints
nia have implemented policies favoring                Materials such as fluoropolymer-                   to reduce their usage and release
reflective coatings for buildings. Similar            based binders could enhance reflec-                into the environment, would make
policies exist in global hotspots such as             tance lifetime and thereby lower                   paints more sustainable.
West and South Asia. Such policies may                year-averaged costs. Soiling poses a
account for PDRC-capable paints as a                  challenge for all PDRC technologies            Additionally, we propose three broader
natural extension of existing cool-roof               as it reduces solar reflectance. Thus,         challenges:
standards and immediately expand                      designs that are resistant to soiling,
their reach. Given these attributes and               such as hydrophobic, biofouling-resis-             (1) Mapping the global geograph-
the optical performance achievable,                   tant topcoats that can withstand phys-             ical scope of radiative cooling
paints emerge as a compelling and                     ical cleaning, could maintain cooling              paints, beyond which cold climates
                                                      performance and lengthen lifetime.                 cause PDRC to increase annual

                                                                                                                    Joule 4, 1–7, July 15, 2020      5
Please cite this article in press as: Mandal et al., Paints as a Scalable and Effective Radiative Cooling Technology for Buildings, Joule (2020),
    https://doi.org/10.1016/j.joule.2020.04.010

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Figure 3. Some Issues Concerning Paints as a Radiative Cooling Technology for Use on a Global Scale
Addressing these issues requires collaboration across a wide range of disciplines, including optics, materials science, meteorology, and policy. The
heatmap on the bottom right was obtained from the Climate Impact Lab website.

     energy usage in buildings.9 Among                   tool,12 where a fraction of roofs across           radiative coolers. Many regions
     factors to be considered are clouds                 the world are painted to raise the                 that stand to greatly benefit from
     and anthropogenic particulates                      earth’s albedo and reduce the climate              radiative cooling technologies also
     (see below), which can be transient                 impact of air conditioning by cooling              see high airborne particulate and
     and hinder both solar and LWIR                      the local environment,9 while pre-                 pollutant levels (e.g., South Asia;
     transmission, as well as future varia-              venting weather disruptions that may               Figure 3). With the growing use of
     tions of meteorological variables                   arise from large-scale, centralized                PDRC technologies, evaluating the
     with climate change. This can aid                   geoengineering. On a smaller scale,                relation between PDRC perfor-
     resource allocation by private and                  such an approach may also mitigate                 mance and pollution and dust
     public sectors in the field.                        urban heat-island effects.                         (both airborne and settled on
                                                                                                            PDRC designs), and potential miti-
     (2) Exploration of super-white paints               (3) Studying the effect of pollution               gation strategies (e.g., covering
     as a ‘‘distributed geoengineering’’                 and dust on the performance of                     loose soil with vegetation, filtering

6       Joule 4, 1–7, July 15, 2020
Please cite this article in press as: Mandal et al., Paints as a Scalable and Effective Radiative Cooling Technology for Buildings, Joule (2020),
 https://doi.org/10.1016/j.joule.2020.04.010

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   industrial emissions), can inform              DECLARATION OF INTERESTS                                    hybrid metamaterial for daytime radiative
                                                                                                              cooling. Science 355, 1062–1066.
   policymaking in those regions.                 A patent (PCT/US2016/038190) has
   Related studies for photovoltaic               been granted, and a provisional patent                   7. Raman, A.P., Anoma, M.A., Zhu, L., Rephaeli,
                                                                                                              E., and Fan, S. (2014). Passive
   panels could be a useful guide in              (U.S. 62/596,145) filed related to prior                    radiative cooling below ambient air
   this regard.                                   works cited in the paper. A patent                          temperature under direct sunlight. Nature
                                                                                                              515, 540–544.
                                                  (U.S. 62/980,998) has been filed related
Interdisciplinary Science to Address              to this work. A.P.R. is a founder of Sky-                8. Raman, A.P., Li, W., and Fan, S. (2019).
the Urgent Global Cooling Need                                                                                Generating Light from Darkness. Joule 3,
                                                  Cool Systems Inc., its chief scientific of-                 2679–2686.
Holistically addressing the above chal-
                                                  ficer, and a member of its board. N.Y. is
lenges requires a convergence of                                                                           9. Baniassadi, A., Sailor, D.J., and Ban-Weiss,
                                                  a founder of MetaRe.                                        G.A. (2019). Potential energy and climate
expertise in fields like optics, materials                                                                    benefits of super-cool materials as a rooftop
science, and meteorology. Given the                                                                           strategy. Urban Climate 29, 100495.
intensifying global need for cooling hu-
                                                   1. Mandal, J., Fu, Y., Overvig, A.C., Jia, M., Sun,    10. Levinson, R., and Akbari, H. (2010). Potential
man environments and associated                       K., Shi, N.N., Zhou, H., Xiao, X., Yu, N., and          benefits of cool roofs on commercial
climate issues, an interdisciplinary                  Yang, Y. (2018). Hierarchically porous                  buildings: conserving energy, saving
                                                      polymer coatings for highly efficient passive           money, and reducing emission of greenhouse
approach to improve the already                       daytime radiative cooling. Science 362,                 gases and air pollutants. Energy Efficiency 3,
deployable solution in paints is perhaps              315–319.                                                53–109.

the most practical way forward. While              2. Sun, X., Sun, Y., Zhou, Z., Alam, M.A., and         11. Berdahl, P., Boocock, S.K., Chan, G.C.-Y.,
this piece highlights the exciting poten-             Bermel, P. (2017). Radiative sky cooling:               Chen, S.S., Levinson, R.M., and Zalich, M.A.
                                                      fundamental physics, materials, structures,             (2018). High quantum yield of the Egyptian
tial of paint coatings as passive daytime             and applications. Nanophotonics 6, 997–                 blue family of infrared phosphors
radiative coolers, we hope that it will               1015.                                                   (MCuSi4O10, M = Ca, Sr, Ba). J. Appl. Phys.
                                                                                                              123, 193103.
spur further research that will establish          3. Zhao, D., Aili, A., Zhai, Y., Xu, S., Tan, G.,
                                                      Yin, X., and Yang, R. (2019). Radiative sky
super-white paints as a standard                      cooling: Fundamental principles, materials,
                                                                                                          12. Munday, J.N. (2019). Tackling Climate
                                                                                                              Change through Radiative Cooling. Joule 3,
approach for radiative cooling of build-              and applications. Appl. Phys. Rev. 6,                   2057–2060.
                                                      021306.
ings worldwide.                                                                                           1Department  of Materials Science and
                                                   4. Yu, N., Mandal, J., Overvig, A., and Shi, N.        Engineering, University of California, 410
                                                      (2016). Systems and Methods for Radiative           Westwood Plaza, Engineering V, Los Angeles, CA
ACKNOWLEDGMENTS                                       Cooling and Heating. https://patentscope.           90095, USA
                                                      wipo.int/search/en/detail.jsf?
J.M. acknowledges support from                        docId=WO2016205717.                                 2Department  of Applied Physics and Applied
Schmidt Science Fellows, in partnership                                                                   Mathematics, Columbia University in the City of
                                                   5. Gentle, A.R., and Smith, G.B. (2010).               New York, 500 West 120th St, Mudd 200, New
with the Rhodes Trust, and thanks Profes-             Radiative heat pumping from the Earth using         York, NY 10027, USA
sor Sir Keith Burnett for his valuable feed-          surface phonon resonant nanoparticles.
                                                      Nano Lett. 10, 373–379.                             *Correspondence:
back on the work. A.P.R. acknowledges                                                                     jyotirmoymandal@ucla.edu (J.M.),
                                                   6. Zhai, Y., Ma, Y., David, S.N., Zhao, D., Lou, R.,   aaswath@ucla.edu (A.P.R.)
support from the Sloan Research Fellow-               Tan, G., Yang, R., and Yin, X. (2017). Scalable-
                                                                                                          https://doi.org/10.1016/j.joule.2020.04.010
ship (Alfred P. Sloan Foundation).                    manufactured randomized glass-polymer

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