Nitrogen‐containing carbons (NC) are a class of sustainable materials for selective CO2 adsorption. A versatile concept is introduced to fabricate flexible NC‐based sensor architectures for room‐temperature sensing of CO2 in a one‐step laser conversion of primary films cast from abundant precursors. By the unidirectional energy impact in conjunction with depth‐dependent attenuation of the laser beam, a layered sensor heterostructure with a porous transducer and active sensor layer is formed. Comprehensive microscopic and spectroscopic cross‐sectional analyses confirm the preservation of the high content of imidazolic nitrogen in the sensor. The performance is optimized in terms of material morphology, chemical composition, and surface chemistry to achieve a linear relative resistive response of up to ΔR/R0 = −14.3% (10% of CO2). Thermodynamic analysis yields ΔadsH values of −35.6 and 34.1 kJ·mol−1 for H2O and CO2, respectively. The sensor is operable even in humid environments (e.g., ∆R/R0,RH = 80% = 0.53%) and shows good performance upon strong mechanical deformation.
The development of mobile, noninvasive, and portable
sensor technologies
for diagnostics and emission control is highly demanded. For that
purpose, laser carbonization is studied as a tool to produce responsive
carbon materials from inexpensive organic precursors for the room-temperature
selective detection of volatile organic compounds (VOCs) applicable
in future sensor array-based devices. To increase the response of
intrinsically low-responsive laser-patterned carbons (LP-C) to analytes
in the gas phase, we tested carbonization in the presence of nanoscale
ZnO precursors in primary inks. Following the addition of a zinc salt,
Zn(NO3)2, a noticeable 43-fold increase in the
sensor response (ΔR/R
0 = −21.5% toward 2.5% acetone) was achieved. This effect
is explained by a significant increase in the measurable surface area
up to ∼700 m2·g–1 due to
the carbothermic reduction supported by the in situ formation of ZnO
nanoparticles. Varying Zn concentrations or the addition of as-prepared
ZnO nanorods lead to different surface properties like the surface
area, porosity, and polarity of LP-C. A predominant effect of the
surface polarity on the selectivity toward different analytes of the
sensors during physisorption, e.g., acetone vs toluene, was identified
and tested. The best-performing LP-C sensors were finely characterized
by transmission/scanning electron microscopies and X-ray photoelectron/energy-dispersive
X-ray/Raman spectroscopies.
A large and growing number of applications benefit from simple, fast and highly sensitive 3D imaging sensors. The Focus-Induced Photoresponse (FIP) can achieve 3D sensing functionalities by simply evaluating the irradiance dependent nonlinear sensor response in defect-based materials. Since this advantage is intricately associated to a slow response, the electrical bandwidth of present FIP detectors is limited to a few $${\text{kHz}}$$
kHz
only. The devices presented in this work enable modulation frequencies of 700 kHz and beat frequency detection up to at least 3.8 MHz, surpassing the bandwidth of reported device architectures by more than two orders of magnitude. The sensors achieve a SNR of at least $$\sim 53\;{\text{dB}}$$
∼
53
dB
at $$115\;{\text{cm}}$$
115
cm
and a DC FIP detection limit of 0.6 µW/mm2. The mature and scalable low-temperature a-Si:H process technology allows operating the device under ambient air conditions waiving additional back-end passivation, geometrical fill factors of $$100\%$$
100
%
and tailoring the FIP towards adjustable 3D sensing applications.
Nitrogen-doped carbons (NC) are a class of sustainable materials for selective CO2 adsorption. We introduce a versatile concept to fabricate flexible NC-based sensor architectures for room-temperature sensing of CO2 in a one-step laser conversion of primary coatings cast from abundant precursors. By the unidirectional energy impact in conjunction with depth-dependent attenuation of the laser beam, a layered sensor heterostructure with porous transducer and active sensor layer is formed. Comprehensive microscopic and spectroscopic cross-sectional analyses confirm the preservation of a high content of imidazolic nitrogen in the sensor. The performance was optimized in terms of material morphology, chemical composition, and surface chemistry to achieve a linear relative resistive response of up to ∆R/R0 = -14.3% (10% of CO2). Thermodynamic analysis yields ΔadsH values of -35.6 kJ·mol-1 and 34.1 kJ·mol 1 for H2O and CO2, respectively. The sensor is operable even in humid environments (e.g., ∆R/R0,RH=80% = 0.53%) and shows good performance upon strong mechanical deformation.
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