黃迎港，王桂英

食品流通與包裝

氣體傳感器在食品智能包裝中的應用研究進展

黃迎港，王桂英

（東北林業(yè)大學 a.工程技術學院 b.輕工技術與工程實驗室，哈爾濱 150000）

系統(tǒng)介紹氣體傳感器的種類和應用現狀，以期為氣體傳感器在不同食品智能包裝中的應用提供參考和借鑒。綜述氣體傳感器在水果、蔬菜、海鮮、肉類等智能包裝方面的應用研究進展，分析氣體傳感器在食品智能包裝中應用的局限性及其未來發(fā)展趨勢。當前消費者對食品安全和新鮮度的要求不斷提高決定了氣體傳感器的應用范圍將不斷擴大，并向安全、綠色、無污染的方向不斷發(fā)展。將氣體傳感器用于改善食品安全性和追溯性具有巨大的潛力，具有廣闊的發(fā)展前景，它能夠在食品保質期內跟蹤和監(jiān)測其新鮮度，保證食品的安全性，并有效地促進了食品包裝技術的快速發(fā)展。

食品包裝；氣體傳感器；保鮮包裝；實時監(jiān)測

智能包裝在產品的流通過程中承擔著信息傳遞、存儲和反饋的功能[1]，傳感器作為智能包裝中至關重要組成部分已成為當前研究的熱點。李洪軍等[2]對智能包裝在動物源性食品質量與安全監(jiān)控中應用的研究進行了總結，但并沒有對傳感器在果蔬智能包裝中的應用進行詳細闡述。路玉鳳等[3]分析了傳感器在果蔬品質檢測上的應用，卻僅就電子鼻和圖像識別技術2個方面進行展開。廖愷芯等[4]結合果蔬檢測機理對傳感器在包裝上的應用進行研究歸納并對氣體傳感器進行了分類，但在傳感器研究的最新進展上不夠全面，因此，文中系統(tǒng)介紹氣體傳感器的種類和它在各種食品智能包裝中的應用現狀，以期為氣體傳感器在不同食品智能包裝中的應用提供參考和借鑒。

1 氣體傳感器概述

根據研究方向的不同，智能包裝技術可以分為信息型和功能控制型2種，氣體傳感器作為信息智能包裝中的一種有效載體，它能夠對包裝內環(huán)境中特定氣體敏感并發(fā)生反應，以監(jiān)測包裝內食品的新鮮度，消費者在選購商品時能夠通過包裝上氣體傳感器的變化得到產品的有效信息，以便做出正確選擇[5]。包裝材料的破損、微生物代謝等作用都會使包裝系統(tǒng)內氣體組分發(fā)生很大的變化，氣體傳感器可以通過化學或酶等反應，在標簽上發(fā)生顏色變化，從而起到監(jiān)測產品新鮮度的作用。根據所檢測氣體種類的不同，氣體傳感器可以分為二氧化碳、氧氣、揮發(fā)性含硫化合物、揮發(fā)性含氮化合物和乙烯綜合型氣體指示器等。

2 氣體傳感器監(jiān)測產品新鮮度的機理

氣體傳感器可以通過監(jiān)測二氧化碳和氧氣含量的變化來計算果蔬的呼吸速率，或者通過監(jiān)測乙烯等氣體來分析果蔬的成熟度。它也可以通過識別魚類中產生的揮發(fā)性含氮化合物、肉制品產生的硫化氫等氣體來檢測生鮮類食品的新鮮度，目前氣體傳感器檢測產品新鮮度的機理主要分為以下2種。

1）通過將天然色素或者某種化學試劑制成可以與特定氣體反應的色素染料，染料與基材復合成指示標簽。將指示標簽置于包裝系統(tǒng)內，智能標簽和這些代謝產物進行化學反應，發(fā)生顏色改變等可視變化，起到提示作用。智能指示標簽能夠以成本低的優(yōu)勢應用于果蔬和肉類的品質監(jiān)測。

2）通過氣體傳感器可以識別包裝內的氣體組分，當氣體環(huán)境發(fā)生改變，傳感器能夠通過監(jiān)測轉換成信號反映出產品的新鮮特性，如電子鼻等設備。目前，電氣體傳感器雖然在產品新鮮度的指示領域中具有測試更準確等優(yōu)勢，但這類系統(tǒng)目前絕大多數結構很復雜，需要昂貴的儀器，大量應用在產品包裝中的成本會過高，因此暫時不適合用在銷售包裝中。

3 氣體傳感器在食品智能包裝的應用研究

3.1 水果

在果蔬的智能包裝系統(tǒng)中，氣體傳感器可對水果在成熟過程中釋放的各種特定氣體進行測定，從而判斷水果的成熟度等質量狀態(tài)?；跉怏w傳感器在水果新鮮度監(jiān)測方面的應用研究見表1。Mahajan等[6]開發(fā)了一種小型且靈活的基于傳感器的呼吸計，借助于呼吸計上的電化學傳感器和紅外傳感器，用于連續(xù)地測量草莓中氧氣的含量。早在2004年，新西蘭的P?P Enterprises超級市場推出了Ripe SenceTM洋梨智能包裝，當洋梨成熟后產生芳香氣體，包裝上的智能標簽由紅色變成黃色[7]。Kim等[8]開發(fā)了一種基于甲基紅的由功能油墨直接打印在紙介質上的柔性傳感器標簽，當蘋果成熟釋放出醛時，標簽顏色由黃色變成橙色，最后變成紅色。

表1 基于氣體傳感器在水果新鮮度監(jiān)測的研究

Tab.1 Research on fruit freshness monitoring based on gas sensors

電子鼻是由某種特定識別模式系統(tǒng)和氣體傳感器組成的儀器，由于電子鼻具有氣體選擇性，使得它不僅可以檢測單一氣體也可以檢測混合氣體。此外，電子鼻在監(jiān)測草莓在采后物流過程新鮮度、撞擊損傷程度等方面也得到了廣泛的研究。這些研究均表明，電子鼻技術能夠有效且智能地分析檢測水果的新鮮度。

王順[11]提出了基于視覺和嗅覺多傳感器融合技術的水果成熟度檢測系統(tǒng)，將視覺系統(tǒng)獲取外觀信息和嗅覺傳感器獲取的氣味信息進行數據融合，從而準確無損地檢測水果成熟度。孫雪[12]構建了適用于葡萄冷鏈物流環(huán)境中檢測的氣體傳感器，通過測試物流冷鏈環(huán)境中CO2、O2和SO2氣體濃度來檢測葡萄的品質變化。Deng等[13]將殼聚糖、納米金顆粒等材料制成可對有機磷、甲基和硫磷農藥快速響應的生物傳感器，該傳感器能快速識別有害物質。近幾年也有很多研究者[14]通過提取天然色素制成新鮮度指示標簽對水果進行新鮮度的檢測。

3.2 蔬菜

由于蔬菜的呼吸作用會產生特殊性氣體使得包裝內氣氛環(huán)境發(fā)生變化，因此，可在包裝內使用可視化的指示材料來監(jiān)測生蔬的新鮮程度[15]，基于氣體傳感器在蔬菜新鮮度監(jiān)測方面的應用研究見表2。Lee等[16]開發(fā)了一種以無紡布作為基材片，溴甲酚綠為變色層，低密度聚乙烯薄膜為外層固定染料的新鮮度指示器，該傳感器可有效地檢測二氧化碳的濃度變化，并能通過連接手機來讀取蔬菜的新鮮度。Chen等[17]通過在成膜液中混合甲基紅和溴百里酚藍溶液制備了辨別鮮切青椒新鮮度的智能標簽，隨著在儲存期間包裝中的二氧化碳的濃度增加，智能標簽從黃綠色變?yōu)槌壬?。Meng等[18]將使用化學染料作為指示劑，并與基材混合制備了CO2傳感器，研究發(fā)現隨著蔬菜產生CO2濃度的增加，標簽顏色發(fā)生明顯變化。

表2 基于氣體傳感器在蔬菜新鮮度監(jiān)測的研究

除了可以檢測二氧化碳氣體外，近幾年也有采用檢測硫化氣體[19]來測試蔬菜新鮮度的方法。此外電子鼻也能夠智能有效地監(jiān)測生蔬的新鮮度[20]，并且氣體傳感器在蔬菜中的農藥殘留病變[21]等方面也有了部分研究，切實保障了食品的安全性。

3.3 海鮮

海鮮類產品含有豐富的蛋白質，營養(yǎng)豐富，但在加工、流通和銷售過程中極易發(fā)生腐敗，因此，研究海鮮類產品新鮮度監(jiān)測技術具有廣闊的發(fā)展前景。海產品的品質變化可以通過在檢測它產生的揮發(fā)性鹽基氮（Tolal Volatile Basic Nitrogen，TVBN）的濃度來判定，隨著TVBN的含量增加會改變環(huán)境的pH值，因此，pH指示劑在海產品的包裝應用中具有巨大的潛力[22]。

3.3.1 蝦類

基于天然色素的氣體傳感器在蝦類新鮮度監(jiān)測方面的應用研究見表3。Liu等[31]通過流延法制備了一種基于姜黃素、黑枸杞花青素和κ–卡拉膠基質的智能包裝膜。在蝦的儲存過程中，隨著TVBN值的升高，包裝膜顏色由淺灰色先變藍綠色再變黃。黃佳茵等[32]以改性聚乙烯醇（Polyvinyl Alcohol, PVA）和甲基纖維素（Methyl Cellulose, MC）作為成膜基材，甲基紅和溴甲酚紫作為指示劑制備指示膜，并對南美白對蝦進行新鮮度監(jiān)測。結果表明在儲存過程中指示膜由紅褐色轉為紫褐色最終變?yōu)楹谏?/p>

除了天然色素以外，Wang等[33]使用了具有高固態(tài)發(fā)射的香豆素氫衍生物來制作了新型比色傳感器。目前，采用電子鼻技術監(jiān)測鮮蝦新鮮度的研究較少[34]，部分學者將熒光物質通過共價鍵鏈接在纖維素分子鏈上來制備熒光傳感器，研究表明該類傳感器具有很高的檢測精度，能夠有效監(jiān)測海鮮的腐敗程度[35]。

3.3.2 魚類

近幾年來，具有成本低、響應快等優(yōu)點的比色陣列傳感器在食品安全領域方面具有巨大的應用潛力。張一冉[36]通過溶膠–凝膠的方法來改善氣敏材料的防水特性并與濾紙結合制備成陣列傳感器來監(jiān)測鱸魚的新鮮度，實驗發(fā)現該傳感器能夠成功識別腐敗的鱸魚從而提高食品安全性。

由于花青素的來源廣泛，易于提取且無毒無害的優(yōu)點使其作為指示劑更容易被人們所接受。一些研究人員從玫瑰茄[37]、紫薯[38]等植物中提取花青素制備指示膜應用于魚類包裝，均起到了很好的指示作用。Zhai等[39]基于玫瑰茄花青素（Roselle Anthocyanins, RACNs）和淀粉/聚乙烯醇（Starch Polyvinyl Alcohol，SPVA）開發(fā)了用于實時監(jiān)測魚肉在冷藏溫度下的新鮮度。隨著魚變質過程中會產生多種堿性揮發(fā)性胺，比色膜隨時間呈現可見的顏色變化，見圖1。目前，基于天然色素作為染料的魚肉新鮮度的氣體傳感器也得到了廣泛的應用，表4列出了相關的研究。

表3 基于天然色素的氣體傳感器在蝦類新鮮度監(jiān)測的研究

Tab.3 Research on the freshness monitoring of shrimp by gas sensors based on natural pigment

除了天然色素外，也有很多化學染料可用于制備新鮮指示劑。Aghaei等[49]使用靜電紡絲技術制備含有茜素的玉米醇溶蛋白納米纖維傳感器來監(jiān)測在4 ℃冷藏條件下虹鱒魚片的品質變化，在儲存5～9 d后傳感器變?yōu)榈仙?，?0～12 d時傳感器的顏色變?yōu)檠蠹t色?；诨瘜W染料的氣體傳感器在魚類新鮮度監(jiān)測的研究見表5。

目前人們通過對數據進行主成分分析（Principal Components Regression, PCA）和線性判別分析（Linear Discriminant Analysis, LDA），并結合揮發(fā)性鹽基氮、菌落總數和三甲胺含量的變化進行分析，可以建立一種利用電子鼻技術判別魚類新鮮度的方法。這類技術在魚肉腐敗檢測中已有了不少的研究[56]。此外，Chung等[57]開發(fā)了一種使用高頻射頻識別（High Frequency Radio Frequency Identification, HF RFID）技術的近端無電池智能傳感器標簽，該系統(tǒng)可通過測量魚的儲存溫度和H2S或NH3氣體的濃度，能夠有效監(jiān)測魚肉的腐敗過程。

圖1 比色膜在4 ℃下165 h內貯藏鰱魚過程中的相應顏色變化

表4 基于天然色素的氣體傳感器在魚類新鮮度監(jiān)測的研究

Tab.4 Research on fish freshness monitoring by gas sensors based on natural pigment

表5 基于化學染料的氣體傳感器在魚類新鮮度監(jiān)測的研究

Tab.5 Research on fish freshness monitoring by gas sensors based on chemical dyes

3.4 肉類

肉類含有豐富的優(yōu)質的蛋白質、脂肪、碳水化合物等營養(yǎng)物質，是人們日常能量攝入的主要來源之一。新鮮肉類在運輸流通的環(huán)節(jié)中容易受到微生物的作用發(fā)生腐敗變質。目前消費者更易接受在流通過程中與肉類產生的微生物代謝特征產物發(fā)生反應的氣體傳感器，該傳感器能夠準確地提供肉類產品的新鮮度信息[58]。

3.4.1 豬肉

對鮮豬肉新鮮度指標的判定，主要從感官、理化和微生物等幾個方面的變化來評價豬肉的新鮮度[59]。在國內豬肉品質的監(jiān)測中已有了很多學者以化學染料作為pH指示劑來制備新鮮度指示卡。胡云峰等[60]選用溴甲酚紫作為pH指示劑，并以棉質纖維紙為基材制備了智能指示紙，研究發(fā)現隨著豬肉腐敗過程的加劇，指示紙的顏色由淺黃色變成深紫色。此外，Chen等[61]開發(fā)了一種由瓊脂（Agar, AG）和ZnTPPS4組成的豬肉新鮮度比色指示劑，室溫（25 ℃）試驗表明，隨著TVBN濃度的升高，標簽的顏色發(fā)生顯著變化。Li等[62]開發(fā)了一種基于釕納米顆粒的H2S納米仿生傳感器，該傳感器對H2S具有特定的快速響應，能夠在線性范圍（0～1 800 nM）內現場監(jiān)測豬肉的新鮮度?；谔烊簧氐臍怏w傳感器應用于豬肉新鮮度監(jiān)測的研究見表6，將花青素作為天然pH指示劑并結合不同的基材可以制備出多種純天然有效的豬肉新鮮度指示標簽。

表6 基于天然色素的氣體傳感器在豬肉新鮮度監(jiān)測的研究

Tab.6 Research on pork freshness monitoring by gas sensors based on natural pigments

電子鼻系統(tǒng)可以對豬肉進行揮發(fā)性鹽基總氮檢測，它可以快速準確地預測出豬肉在貯藏期間的品質變化，從而監(jiān)測豬肉的新鮮度[69]。此外，Song等[70]首次使用廢棄的蔥根作為生物模板制造了SnO2微管，它在低能耗的情況下便能準確檢測高濕大氣下的H2S氣體，因此該傳感器在鮮豬肉檢測方面極具應用價值。Shi等[71]基于二氧化鈦聚苯胺/絲素纖維開發(fā)了一種新型低成本微型傳感器，該傳感器的輸出響應值與豬肉中的TVBN水平顯示出良好的相關性。

3.4.2 雞肉

基于氣體傳感器在雞肉新鮮度監(jiān)測的研究見表7。早在1995年，Otto等[72]在雞肉的包裝材料上涂覆作為指示劑的硝酸鉛乳液，指示劑會與雞肉腐敗產生的H2S發(fā)生反應，由棕色變?yōu)楹谏?。Liang等[73]使用沙蒿膠、紅甘藍花青素和羧甲基纖維素鈉制備了一種智能指示膜，該薄膜隨著NH3濃度的升高，顏色由黃綠色變?yōu)辄S色。

表7 基于氣體傳感器在雞肉新鮮度監(jiān)測的研究

Tab.7 Research on chicken freshness monitoring based on gas sensors

Koskela等[76]利用柔性印制電路板的技術，以醋酸銅印刷紙為原料，在基板上制成了一種用于監(jiān)測雞肉新鮮度的氣體傳感器。實驗證明，氣體傳感器對雞肉腐敗產生的H2S具有良好的響應。Lee等[77]開發(fā)了一種由內部聚醚嵌段酰胺、8種聚合物固定的pH染料變色層和外部聚對苯二甲酸乙二醇酯組成的比色陣列新鮮度指示器，為雞肉新鮮度的監(jiān)測提供一種低成本的方法。

3.4.3 牛肉

基于氣體傳感器在牛肉新鮮度監(jiān)測的研究見表8。Mehdizadeh等[78]以石榴皮提取物、百里香精油和殼聚糖–淀粉制備了復合膜，并探究智能膜對4 ℃下儲藏21 d牛肉貨架期的影響，發(fā)現制得的復合薄膜具備更好的抗菌和力學性能，并能夠延長牛肉的貨架期。Ezati等[79]通過在纖維素–殼聚糖膜中摻入茜素制成了比色指示膜，當牛肉腐敗時的總揮發(fā)性堿性氮（TVBN）達到臨界值時，指示膜顯示出從棕色到紫色的顏色變化。

翟曉東[81]利用熒光共振能量轉移效應，制備了具有雙發(fā)射特點的硅量子點–銀納米簇智能指示膜，在牛肉的腐敗過程中，指示膜與硫化氫和甲硫醇發(fā)生反應，顏色由紅色變成藍色。此外電子鼻技術在監(jiān)測牛肉新鮮度、分析燉煮牛肉的風味[82]、辨別摻假牛肉[83]等方面也有了部分研究。

3.4.4 羊肉

基于氣體傳感器在羊肉新鮮度監(jiān)測的研究見表9。孫武亮[84]將染料通過靜電紡絲技術制備了能夠響應羊肉新鮮度的納米纖維膜，發(fā)現其對冷鮮羊肉貯藏期間的品質有了很好的監(jiān)測。Alizadeh-sani等[85]通過將伏牛花花色苷與甲基纖維素/殼聚糖納米纖維復合膜混合制備了pH指示膜，當羊肉腐敗時，薄膜由粉色變成無色。

表8 基于氣體傳感器在牛肉新鮮度監(jiān)測的研究

Tab.8 Research on beef freshness monitoring based on gas sensors

表9 基于氣體傳感器在羊肉新鮮度監(jiān)測的研究

Tab.9 Research on mutton freshness monitoring based on gas sensors

此外王綪等[90]、張宗國等[91]將電子鼻結合頂空氣相色譜–離子遷移譜（Gas Chromatographyion Mobility Spectrometry，GC-IMS）技術對摻了鴨肉的假羊肉進行定性辨別，實驗表明電子鼻能夠準確地區(qū)分不同摻假比例的羊肉樣品，說明該技術可為摻了鴨肉的假羊肉的檢測提供良好的技術支撐。

3.5 其他食品

3.5.1 泡菜

泡菜這類發(fā)酵類產品中，CO2是微生物生長過程中的主要代謝產物，因此，CO2含量的上升標志著食品新鮮度的下降[92]。Hong等[93]制備了用于指示韓國泡菜的新鮮度的pH指示薄膜，研究發(fā)現在泡菜發(fā)酵的過程中，二氧化碳濃度逐漸升高，從而使包裝內環(huán)境的酸性增強，薄膜顏色會發(fā)生明顯變化，對泡菜的品質起到了監(jiān)測的作用。Baek等[94]制備并表征了具有pH依賴性的聚醚嵌段酰胺膜型CO2指示器，其中包含了甲基紅和溴百里酚藍指示劑染料。在泡菜初始發(fā)酵階段，指示器為藍色，最佳發(fā)酵期間為黃色，發(fā)酵結束時為紅色，實現了在儲存期間對包裝內泡菜的實時監(jiān)控。

3.5.2 甜品

Nopwinyuwong等[95]通過在尼龍/線性低密度聚乙烯膜上流延并涂覆溴麝香草酚藍和甲基紅，制備用于實時監(jiān)測甜點新鮮度的指示標簽，隨著甜品中二氧化碳濃度的不斷增加，指示標簽從綠色變?yōu)槌壬ňG色表示新鮮、橙色表示變質），見圖2。邢月等[96]開發(fā)了一種基于聚乳酸、溴百里香酚藍和甲基紅的新鮮度指示卡，用于監(jiān)測饅頭、面包等面食的新鮮度。當食品發(fā)生腐敗時，指示卡由綠色變?yōu)辄S色，最終變?yōu)槌燃t色。Pisuchpen[97]研制了一種基于甲基紅和溴百里酚藍混合染料的CO2指示標簽，用來監(jiān)測和指示泰國傳統(tǒng)甜品Thong–EK的保質期。在儲存過程中隨著CO2含量的增加，指示標簽由藍色逐漸變成綠黃色、綠色，最后變成黃色。

圖2 Nopwinyuwong開發(fā)的用于實時監(jiān)測甜食新鮮度的指示標簽

3.5.3 乳類食品

在乳類食品中，乳酸菌的發(fā)酵會產生CO2，因此乳類食品的新鮮度監(jiān)測主要也是通過pH指示劑監(jiān)測包裝內的CO2的濃度來實現的。當食品腐敗過程釋放出CO2時，包裝上的pH指示劑會隨著包裝內環(huán)境pH值的降低發(fā)生明顯的顏色變化[98]?；谔烊簧氐臍怏w傳感器在牛奶新鮮度監(jiān)測的研究見表10。

表10 基于天然色素的氣體傳感器在牛奶新鮮度監(jiān)測的研究

Tab.10 Research on milk freshness monitoring by gas sensors based on natural pigments

王帥等[105]開發(fā)了一種基于無線射頻識別技術的低功率pH傳感器，該傳感器可應用于對O2和CO2氣體敏感的牛奶和肉類的包裝中，以實時監(jiān)測其新鮮度的變化。此外，具有高靈敏性和客觀性的電子鼻技術在牛奶的風味檢測[106]、安全性檢測[107]和貨架期預測[108]中均有了很多的研究應用，電子鼻技術在實現奶類制品的檢測的同時保證了奶類制品的品質。

4 結語

氣體傳感器作為智能包裝的分支能夠在提高包裝智能化和信息化的同時也滿足了人們對于食品安全性的需求。目前，氣體傳感器在不同的食品上已有了廣泛的應用，它的應用與發(fā)展為產品的質量和安全提供了可靠的保障，但是對智能包裝中的活性與智能成分的毒理學的研究還不夠全面，許多應用在氣體傳感器中的化學成分較為復雜，也存在很多人工合成的物質成分，它的安全性還不能得到保證，智能包裝的高成本也阻礙了氣體傳感器的應用，因此，需要更多地去探究低成本的天然物質應用于氣體傳感器的可行性，以發(fā)揮氣體傳感器在改善食品安全性和可追溯性的巨大潛力，推動該項智能技術的發(fā)展，使智能包裝技術具有更廣闊的前景。

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Research Progress of Gas Sensors in Smart Food Packaging

HUANG Ying-gang, WANG Gui-ying

(a. College of Engineering and Technology b. Light Industry Technology and Engineering Laboratory,Northeast Forestry University, Harbin 150000, China)

The work aims to sysmetaically introduce the type and application status of gas sensors, so as to provide experience and reference for the application of gas sensors in different smart food packaging. The application research progress of gas sensors in smart packaging of fruits, vegetables, seafood, meat, etc. was reviewed and the limitations of the application of gas sensors in smart food packaging and the future development trends were analyzed. The current consumers’ increasing requirements for food safety and freshness determined the wide application of gas sensors and made them continue to develop in a safe, green, and pollution-free direction. The application of gas sensors in improving food safety and traceability has great potential and broad development prospects. The gas sensors can track and monitor the freshness of food during the shelf life, ensure food safety, and effectively promote the development of food packaging technology.

food packaging; gas sensors; fresh-keeping packaging; real-time monitoring

TS206

A

1001-3563(2022)15-0137-13

10.19554/j.cnki.1001-3563.2022.15.016

2021–12–29

國家自然科學基金面上項目（32071685）；黑龍江省自然科學基金資助項目（LH2019E001）；黑龍江省自然科學基金聯(lián)合引導項目（LH2019C002）

黃迎港（1997—），女，東北林業(yè)大學碩士生，主攻智能包裝材料成型技術。

王桂英（1968—），女，博士，東北林業(yè)大學副教授，主要研究方向為輕工技術裝備及自動化、智能包裝技術。

責任編輯：曾鈺嬋