What the published science already showed.
Before I get to the absurd part, let me lay out what the public record looked like by 2021.
Holtus 2018 · Nature Chemistry · the inventor's own paper
This is the paper that quietly destroys every novelty argument the applicant could ever make. Lukas Helmbrecht, the first-named inventor on the patent, is a co-first author. Willem Noorduin, the corresponding author on the patent and the founder of Lumetallix, is the corresponding author on this paper too. See the author byline yourself, highlighted on page 1. The paper's Supplementary Information section 6, page 7 contains the recipe:
"To convert the surface of a sand dollar a solution of
25 mg methyl ammonium bromide in 2.5 g of isopropanol was prepared. The solution was then
applied onto the sand dollar shell using a Pasteur pipet. When the conversion reaction was performed under UV radiation, the formation of the perovskite can be
observed in real-time. The initially white sand dollar turns light orange in daylight and
fluoresces bright green under UV irradiation."
Holtus 2018, Supplementary Information, Section 6, page 7. See it for yourself · highlighted.
And from page 2 of the same supplementary information, describing the actual published movie file:
"Real-time movie of the conversion of a 3.5 cm sized sand dollar into CH₃NH₃PbBr₃ by dripping a CH₃NH₃Br solution on the PbCO₃ converted sand dollar surface under UV illumination at 365 nm."Holtus 2018, Supplementary Information, page 2 · Movie 1 description.
That formulation is methylammonium bromide at 1% in isopropanol, applied as drops on a real-world solid lead-bearing substrate, illuminated with 365 nm UV, producing real-time green fluorescence. That is the formulation of the FluoroSpec product I sell today, give or take a tenth of a percent. That is the formulation of the Lumetallix product they sell today, give or take a tenth of a percent. The patent application's stock solution at paragraph [0076] is 1.6% in isopropanol. The recipe was published in 2018. By the inventors. In Nature Chemistry. With supplementary information. With a movie file.
Yan 2019 · Scientific Reports · MABr as a lead-detection method, naked-eye
While the AMOLF group was sitting on what to do with their 2018 chemistry paper, a different team published the chemistry as an explicit lead-detection method. Yan et al. (2019) in Scientific Reports showed the same MABr-and-UV reaction working on paper test strips. From page 5 of their paper:
"The letters 'BJTU' were written with PbBr₂ solution (0.1 M) on paper strips. The 'BJTU' are invisible on paper strips under ambient light. However, after loading of MABr solutions (0.8 M) on these paper strips, the fluorescent letters under UV illumination can be observed by the naked eye."
Yan 2019, pages 5–6. See it for yourself · highlighted.
That is the demonstration. PbBr₂ on paper, MABr on top, UV light, green letters visible to the unaided eye. As a proof of using this chemistry to find lead, that is the whole idea, written down in 2019, two years before the patent's priority date. Yan also reports a detection limit of 1.6 × 10⁻³ M PbBr₂, which on a paper strip works out to nanogram-scale total lead.
This paper alone was enough for the U.S. examiner. Every claim of the U.S. patent application was rejected over Yan + Kayano. The examiner did not even need to reach for the inventor's own paper. The published Yan reference, plus a generic teaching about lead in electronics, was sufficient.
Wang 2021 · Sensors and Actuators B · 5 ppb on a 13 mm disk in 50 mL of water
Then there is Wang et al. (2021) in Sensors and Actuators B. This paper, published months before the patent's priority date, used the same chemistry to detect lead bound onto a sulfhydryl-functionalized mesoporous alumina film. The numbers, straight from the abstract:
"the Pb(II) adsorption capacity of the sulfydryl functionalized film was found to be drastically enhanced after sulfydryl modification. Under the optimal conditions, the Pb(II) adsorption capacity of the sulfydryl functionalized film was estimated to be
94.9 µg/g... a limit of detection (LOD)
as low as 5 × 10⁻³ µg/mL was achieved."
Wang 2021, abstract. See it for yourself · highlighted.
That LOD is 5 × 10⁻³ micrograms per milliliter. Five parts per billion in water. They achieved this on a 13 mm diameter mesoporous alumina film immersed in 50 mL of water at 55°C for 25 minutes, then dropped 20 µL of MABr solution on the film, dried it, and looked at it under 365 nm UV. From page 4:
"The LOD for Pb(II) determination was found to be 5 × 10⁻³ µg/mL evaluated by the typical 3-times of signal to noise method... The sensitivity of this method meets the requirement for Pb(II) determination in drinking water samples following the National Test Standard of China GB 5749–2006, in which a maximum level of Pb(II) should be lower than 0.01 µg/mL."
Wang 2021, page 4. See it for yourself · highlighted.
The 0.01 µg/mL standard they reference is also the WHO drinking water guideline and the U.S. EPA limit. Wang's published method, in 2021, hit twice that sensitivity. On a closed substrate. On bound lead. On a thirteen-millimeter disk in fifty milliliters of water. The LOD is the most rigorous metric in analytical chemistry. They reported it. They measured it. They published it in a peer-reviewed journal months before the patent claimed priority.
And here is the part that actually matters for the patent argument. The European patent application's most recent argument hinges on the idea that real-world lead is somehow "embedded in the structure of the material" and "not present in the form of free Pb ions in a freely accessible form" and therefore unexpectedly hard to detect with this chemistry. Wang's substrate is exactly the kind of substrate the EP attorneys say is too closed for the chemistry to work on. A solid mesoporous alumina film with lead bound to sulfhydryl ligands embedded in its surface. The lead is not free. The substrate is not open. And the chemistry works on it at five parts per billion. That paper has been on the patent's information disclosure statement since prosecution started.
Zang 2017 · Solar Energy Materials · PbO converts the same way
Zang et al. (2017) showed lead oxide reacting directly with methylammonium-halide reagent in isopropanol to form methylammonium-lead-iodide perovskite. This matters because lead in old paint and lead in glaze is mostly not free Pb²⁺. It is mostly basic lead carbonate (white lead, the historical pigment) and lead oxide (in glazes, in oxidized solder). The Zang result tells us all of these substrates feed into the same chemistry. None of this is news to anyone who has read the perovskite-synthesis literature. The Lumetallix application has Zang on its own information disclosure statement.
So by April 2021, the published record showed: the chemistry, the formulation, the application method, the substrate generality, and explicit demonstrations of using it as a lead-detection method on solid surfaces. That was the world the patent application was filed into.