As one of the most toxic forms of arsenic, inorganic As(III) is easy to accumulate in rice, leading to severe public health problems. Effective control of As(III) requires the development of fast analytical methods for its detection with high sensitivity and specificity. Toward this end, in this work, we report the fabrication of an As(III) electrochemical sensor based on a solution-gated graphene transistor (SGGT) platform with a novel sensing mechanism. The gold gate electrode of the SGGT was modified with DNA probes and then blocked with bovine serum albumin (BSA). The specific interaction between As(III) and gold disrupted the adsorption states of DNA probes, redistributing surface charges on the gate electrode, further leading to potential drop changes at the interfaces of the gate electrode and graphene active layer. This new mechanism based on DNA-charge-redistribution-induced SGGT current responses (denoted as "DNA-SGGT") was found to greatly improve the selectivity of the sensor: the response of DNA-SGGT to As(III) was effectively enhanced fourfold, while to other interfering cations, it was significantly reduced. The optimized sensor showed a detection limit as low as 5 nM with superior selectivity to As(III). The as-prepared DNA-SGGT-based sensor has also been successfully applied to the detection of As(III) in practical rice samples with a high recovery rate, showing great potential for heavy metal detection in many types of food samples.
Keywords: DNA-gated graphene transistor; arsenic; biosensor; electrochemistry; rice.