In this work, a TFB (poly[(9,9-dioctylfluorenyl-2,7-diyl)-co-(4,4'-(N-(4-s-butylphenyl)diphenylamine)]) sensor with a cylindrical nanopore structure exhibits a high sensitivity to ammonia in ppb-regime. The lifetime and sensitivity of the TFB sensor were studied and compared to those of P3HT (poly(3-hexylthiophene)), NPB (N,N'-di(1-naphthyl)-N,N'-diphenyl-(1,1'-biphenyl)-4,4'-diamine), and TAPC (4,4'-cyclohexylidenebis[N,N-bis(4-methylphenyl) benzenamine]) sensors with the same cylindrical nanopore structures. The TFB sensor outstands the others in sensitivity and lifetime and it shows a sensing response (current variation ratio) of 13% to 100 ppb ammonia after 64 days of storage in air. A repeated sensing periods testing and a long-term measurement have also been demonstrated for the test of robustness. The performance of the TFB sensor is stable in both tests, which reveals that the TFB sensor can be utilized in our targeting clinical trials. In the last part of this work, we study the change of ammonia concentration in the breath of hemodialysis (HD) patients before and after dialysis. An obvious drop of breath ammonia concentration can be observed after dialysis. The reduction of breath ammonia is also correlated with the reduction of blood urea nitrogen (BUN). A correlation coefficient of 0.82 is achieved. The result implies that TFB sensor may be used as a real-time and low cost breath ammonia sensor for the daily tracking of hemodialysis patients.
Point-of-care (POC) application for monitoring of breath ammonia (BA) in hemodialysis patients have emerged as a promising non-invasive health monitoring approach. In this context, many organic gas sensors have been reported for BA detection. However, one of the major challenges for its integration with portable POC application is to achieve long lifetime and high operational current at low voltage. Herein, we propose a double active layer (DL) strategy that exploits an ultra-thin layer of Poly(3hexylthiophene-2,5-diyl) (P3HT) to serve as a work function buffer, combined with an acceptor-donor polymer Poly [[4,8-as a new sensing material. We show that the DL sensor exhibits a sustainable enhanced operational current of microampere level and a stable sensing response even with the presence of P3HT layer. This effect is carefully examined with different aspect, including vertical composition profile of DL configuration, lifetime testing on different sensing layer, morphological analysis, and the versatility of the DL strategy. Finally, we utilize the CT/P3HT-DL sensor to conduct a long-term tracing of BA concentration in two hemodialysis (HD) patients before and after HD, and correlate it with the blood urea nitrogen (BUN) levels. A good correlation coefficient of 0.96 is achieved. The result demonstrates the potential of this DL strategy to be used to integrate organic sensor in POC devices.
Previous studies have shown that breath ammonia (breath-NH3) concentration is associated with blood urea nitrogen (BUN) levels. However, interindividual variations in breath-NH3 concentrations were observed. Thus, the present study aimed to assess the effect of oral cavity conditions on breath-NH3 concentration and to validate whether the measurement of breath-NH3 concentration is feasible in clinical settings. A total of 125 individuals, including patients with stage 3 to 5 chronic kidney disease (CKD3–5), those on dialysis, and healthy participants, were recruited. A nanostructured sensor was used to detect breath-NH3 concentrations. Pre- and post-gargling as well as pre- and post-hemodialysis (HD) breath-NH3, salivary pH, and salivary urea levels were measured. Breath-NH3, salivary urea, salivary pH, and BUN levels were positively correlated to each other. Breath-NH3 concentrations were associated with BUN levels (r = 0.43, p < 0.001) and were significantly higher in CKD3–5 (p < 0.005) and dialysis patients (p < 0.001) than in healthy participants. Higher correlation coefficients were noted between breath-NH3 concentrations and BUN levels during follow-up (r = 0.59–0.94, p < 0.05). When the cutoff value of breath-NH3 was set at 523.65 ppb, its sensitivity and specificity in predicting CKD (BUN level >24 mg dl−1) were 87.6% and 80.9%, respectively. Breath-NH3 concentrations decreased after HD (p < 0.001) and immediately after gargling (p < 0.01). Breath-NH3 concentration, which was affected by gargling, was correlated to BUN level. The measurement of breath-NH3 concentration using the nanostructured device may be used as a tool for CKD detection and personalized point-of-care for CKD and dialysis patients. The current study had a small sample size. Thus, further studies with a larger cohort must be conducted to validate the effect of oral factors on breath-NH3 concentration and to validate the benefit of breath-NH3 measurement.
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