本文選題：光尋址電位傳感器 + 光電集成微納傳感器芯片�。� 參考：《浙江大學(xué)》2014年博士論文

【摘要】：伴隨著經(jīng)濟(jì)發(fā)展和人類進(jìn)步,人們尋求一種更為良性循環(huán)的、可持續(xù)發(fā)展的生活方式。環(huán)境污染、食品安全、醫(yī)療水平與人體健康密切相關(guān),成為了人們?nèi)粘Ｉ钪嘘P(guān)注的重中之重。同時(shí),這些領(lǐng)域衍生的科學(xué)研究也逐漸對(duì)無(wú)損、快速、智能檢測(cè)技術(shù)提出了更高的要求。人工電子舌以其快速、低功耗、智能化、易操作、價(jià)格低廉、便攜化程度高的優(yōu)點(diǎn),近年來(lái)成為了研究的熱點(diǎn)和實(shí)用的實(shí)時(shí)在線檢測(cè)手段,并被廣泛地應(yīng)用于環(huán)境檢測(cè)、食品、醫(yī)學(xué)、藥物分析等領(lǐng)域。 本文以離子敏電位型電子舌中的光尋址電位傳感器和離子選擇性電極為主要的研究對(duì)象,并結(jié)合細(xì)胞阻抗傳感器,考察了其在水環(huán)境重金屬監(jiān)測(cè)和藥物苦味及藥效評(píng)價(jià)中的應(yīng)用。在半導(dǎo)體物理學(xué)基礎(chǔ)上,設(shè)計(jì)并研制了一種新型結(jié)構(gòu)的重金屬光尋址電位傳感器敏感陣列,實(shí)現(xiàn)了傳感器內(nèi)部微型集成化和水樣多參數(shù)檢測(cè)。綜合伏安電流型電子舌中的微電極陣列和納米帶電極陣列,設(shè)計(jì)了兩種光電復(fù)合微納傳感器芯片,實(shí)現(xiàn)了多傳感器微型集成化和水環(huán)境監(jiān)測(cè)無(wú)線傳感器網(wǎng)絡(luò)節(jié)點(diǎn)的功能。針對(duì)離子選擇電極在藥物苦味評(píng)價(jià)中的應(yīng)用,探究了用于中西藥苦味物質(zhì)檢測(cè)的敏感機(jī)理、電極篩選方案、藥物苦味預(yù)測(cè)和掩味劑的苦度抑制效果評(píng)價(jià)。基于細(xì)胞阻抗傳感器,對(duì)中藥的藥效進(jìn)行了定量分析。研究工作受國(guó)家高技術(shù)研究發(fā)展計(jì)劃(863計(jì)劃)項(xiàng)目、國(guó)家重點(diǎn)基礎(chǔ)研究發(fā)展計(jì)劃(973計(jì)劃)項(xiàng)目和國(guó)家基金委國(guó)家合作專項(xiàng)的支持。 本文所做的主要工作和創(chuàng)新如下： 1.提出了一種基于PVC薄膜敏感材料的光尋址電位傳感器的設(shè)計(jì)方法,并將其應(yīng)用于水環(huán)境重金屬的檢測(cè)中。 基于薄膜加工工藝,設(shè)計(jì)并制造了聚氯乙烯薄膜LAPS、可對(duì)水樣中的Zn2+、Cd~(2+)、Pb~(2+)、Cu~(2+)進(jìn)行測(cè)定。對(duì)成膜效果進(jìn)行了表征,通過(guò)溶液標(biāo)定測(cè)試了傳感器的靈敏度,穩(wěn)定性,選擇性,檢測(cè)下限和響應(yīng)時(shí)間等電化學(xué)特性參數(shù)。進(jìn)一步考察了硅烷化表面修飾在改善表面水合特性和降低表面對(duì)H+敏感度方面的效果,以及支持電解質(zhì)在阻抗匹配,調(diào)節(jié)溶液總陽(yáng)離子濃度平衡,保證測(cè)試溶液穩(wěn)定性以優(yōu)化測(cè)試條件方面的意義。 2.設(shè)計(jì)了一種新型重金屬檢測(cè)的LAPS陣列傳感器,解決了重金屬檢測(cè)中的噪聲串?dāng)_問(wèn)題,提高了傳感器的穩(wěn)定性和響應(yīng)速度。 在該傳感器的制備工藝中,對(duì)非敏感區(qū)域進(jìn)行了重?fù)诫s和表面生長(zhǎng)厚氧化層的處理,以此降低其內(nèi)部串?dāng)_對(duì)敏感區(qū)域的影響。同時(shí),在敏感區(qū)域表面成膜構(gòu)建多敏感陣列實(shí)現(xiàn)LAPS內(nèi)部集成化。經(jīng)過(guò)實(shí)際測(cè)試,同傳統(tǒng)的LAPS傳感器陣列相比,新型結(jié)構(gòu)LAPS陣列具有很高的噪聲串?dāng)_抑制比,更高的穩(wěn)定性和更快的響應(yīng)時(shí)間。PVC與ChG混合敏感陣列的各敏感單元在10-5-10-1mol/L濃度范圍的響應(yīng)電位均在28-30mV之間,響應(yīng)時(shí)問(wèn)在3-10s,線性區(qū)間在10-5-10-1mol/L,檢測(cè)下限在10-6mol/L左右。PVC薄膜對(duì)特定離子具有很好的選擇特異性但壽命相對(duì)較短,而ChG薄膜雖然受部分干擾離子的影響,但其使用壽命相對(duì)較長(zhǎng)。 3.提出了一種重金屬超低濃度檢測(cè)的緩沖體系,明顯降低了重金屬濃度的檢測(cè)下限。 傳感器選用pH-LAPS與重金屬LAPS的集成敏感陣列,使用重金屬離子溶液、絡(luò)合劑、pH緩沖溶液和總離子濃度調(diào)節(jié)劑配置重金屬超低濃度緩沖體系。實(shí)測(cè)結(jié)果顯示,兩種重金屬離子敏感單元對(duì)Cd2+和Pb2+在10-18-10-6M的范圍內(nèi)標(biāo)定曲線的靈敏度分別為29.7mV/pCd和29.3mV/pPb,線性相關(guān)系數(shù)分別為0.9842和0.9913。緩沖溶液和非緩沖溶液體系下的標(biāo)定曲線在聯(lián)立下可保持很好的線性相關(guān)性,傳感器在重金屬離子緩沖溶液中的檢測(cè)下限也可以一直被延續(xù)到皮摩爾的級(jí)別,達(dá)到了超低濃度。 4.深入研究了光尋址電位傳感器與微納電極復(fù)合的集成傳感器芯片設(shè)計(jì)方法,初步實(shí)現(xiàn)了光電與電化學(xué)傳感器的相互校準(zhǔn)功能。 結(jié)合光電集成微納傳感器芯片,在同一個(gè)硅基底上,分別實(shí)現(xiàn)了LAPS與MEA, LAPS與NEA的多傳感器集成化思路。并基于該復(fù)合芯片,配套設(shè)計(jì)了微流控表面封裝、流動(dòng)注射分時(shí)檢測(cè)系統(tǒng)以及水環(huán)境無(wú)線傳感器監(jiān)測(cè)網(wǎng)絡(luò)。通過(guò)建立多元回歸方程組,對(duì)多傳感單元檢測(cè)的數(shù)據(jù)進(jìn)行融合和訓(xùn)練,實(shí)現(xiàn)了傳感器系統(tǒng)片上的自校準(zhǔn)。 5.通過(guò)與俄羅斯的國(guó)際合作探索了電子舌與新型的細(xì)胞傳感器相結(jié)合用于藥物苦味和藥效評(píng)價(jià)的方法。 基于電子舌系統(tǒng),對(duì)8種西藥苦味API成分的苦度進(jìn)行預(yù)測(cè),以及考察加入甜味物質(zhì)對(duì)API以及藥物苦度的抑制效果。此外,本文首次提出了將電子舌用于中藥湯劑的苦度評(píng)價(jià)預(yù)測(cè)體系中。選取8種中藥飲片、1種中藥復(fù)方以及鹽酸小檗堿制成湯劑進(jìn)行檢測(cè),采用PCA分析響應(yīng)電位數(shù)據(jù)矩陣,對(duì)不同類型的中藥湯劑進(jìn)行分類。采用PLS對(duì)離子選擇電極的響應(yīng)電位矩陣和人體口嘗評(píng)定的苦度值之間的相關(guān)性進(jìn)行訓(xùn)練,構(gòu)造預(yù)測(cè)模型,采用交叉驗(yàn)證法(留一法)評(píng)價(jià)模型的預(yù)測(cè)能力�；诩�(xì)胞阻抗傳感器,設(shè)計(jì)了中藥的藥效檢測(cè)實(shí)驗(yàn)。結(jié)果表明,麻黃湯和單味甘草湯劑在10μg/mL-200μg/mL的濃度范圍內(nèi)對(duì)Hela細(xì)胞的生長(zhǎng)增殖均表現(xiàn)出促進(jìn)作用,且隨著濃度的增大促進(jìn)作用變強(qiáng)。從細(xì)胞水平上佐證了麻黃湯和甘草促進(jìn)細(xì)胞增殖的功用。
[Abstract]:Along with economic development and human progress , people seek a more virtuous cycle , sustainable development life style . Environmental pollution , food safety , medical level are closely related to human health , and become the focus of people ' s daily life .


On the basis of semiconductor physics , two photoelectric composite micro - nano sensor chips are designed and developed , and two kinds of photoelectric composite micro - nano sensor chips are designed and developed . The research work is supported by the national high - tech research development plan ( 863 plan ) project , the national key basic research development plan ( 973 plan ) project and the national cooperation special support .


The main work and innovations of this paper are as follows :


1 . A design method of an optical addressing potential sensor based on PVC thin film sensitive material is proposed and applied to the detection of heavy metals in water environment .


Based on the thin film processing technology , the paper designs and manufactures the polyvinyl chloride film LAPS , which can be used for the determination of Zn2 + , Cd ~ ( 2 + ) , Pb ~ ( 2 + ) and Cu ~ ( 2 + ) in water sample . The effect of the modification of silanized surface on improving the surface hydration characteristics and reducing the sensitivity of the surface to H + is tested .


2 . A new type of LAPS array sensor for heavy metal detection is designed , which solves the problem of noise crosstalk in heavy metal detection , and improves the stability and response speed of the sensor .


In the preparation process of the sensor , the non - sensitive area is heavily doped and the surface - grown thick oxide layer is processed to reduce the influence of the internal crosstalk on the sensitive area . In addition , the novel structure LAPS array has a high noise crosstalk suppression ratio , a higher stability and a faster response time than the conventional LAPS sensor array .


3 . A kind of buffer system for heavy metal ultra - low concentration detection is proposed , and the lower limit of heavy metal concentration is obviously reduced .


The results show that the sensitivity of the two heavy metal ion sensitive units to the calibration curves in the range of 10 - 18 - 10 - 6M is 29.7mV / pCd and 29.3mV / pPb , and the linear correlation coefficients are 0.9842 and 0.9913 respectively . The calibration curve in the buffer solution and the non - buffer solution system can maintain a good linear correlation . The lower detection limit of the sensor in the heavy metal ion buffer solution can also be extended to the level of the picomolar ratio , and the ultra - low concentration is achieved .


4 . The design method of the integrated sensor chip of photoaddressable potentiometric sensor and micro - nano electrode is studied , and the mutual calibration function of photoelectric and electrochemical sensors is realized .


Combined with the photoelectric integrated micro - nano sensor chip , the multi - sensor integration idea of LAPS and MEA , LAPS and nea is realized on the same silicon substrate . Based on the composite chip , the micro - fluidic surface packaging , the flow injection time - sharing detection system and the water environment wireless sensor monitoring network are designed , and the data detected by the multi - sensing unit is fused and trained by establishing a multiple regression equation system , and self - calibration on the sensor system chip is realized .


5 . The method of combining electronic tongue with new cell sensor for drug bitterness and efficacy evaluation is explored through international cooperation with Russia .


Based on the electronic tongue system , the bitterness of eight kinds of western medicine bitter taste API components was predicted , and the effect of adding sweet substance on API and the bitterness of medicine was studied .
【學(xué)位授予單位】：浙江大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2014
【分類號(hào)】：R318

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本文編號(hào)：1959698