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Carbon-based nanomaterials (CANOMATs), including fullerenes, carbon nanotubes, graphene, and their derivatives, are widely considered to be the next-generation materials for a broad range of biomedical applications, owing to their unique opto-electronic, chemical, and mechanical properties. However, for bio-applications, CANOMATs need to be surface-functionalized, to render them passive, non-toxic, and water-soluble. Here, we review the current state-of-the-art in the methods of functionalization of CANOMATs. In contrast to other Reviews, we present an objective analysis of the various approaches reported in the literature, using metrics such as the agent of functionalization, number of steps, and time required, the need for special instruments, effect on properties, scalability, reproducibility, and applications. Our Review offers a way for researchers to make a rational selection of the process of functionalization to best suit their desired application. This opens up new opportunities for developing targeted functionalization strategies, based on the need to excel at the above metrics. Dr. Neelkanth M. Bardhan (Neel) did his undergraduate in materials science, with a Bachelor of Technology from the Indian Institute of Technology (IIT) Bombay in Mumbai, India. He then did his Ph.D. in Materials Science and Engineering from the Massachusetts Institute of Technology in Cambridge, MA, USA. For his Ph.D. research on the use of biologically templated, carbon-based nanomaterials for biosensing and diagnostic applications, Neel was a recipient of the 2015 MRS Graduate Student Gold Award, awarded by the Materials Research Society in April 2015. Neel is currently a dual fellow, funded by the 2016 Misrock Postdoctoral Fellowship, and the RLE Translational Fellows Program, working toward clinical translation of his nanotechnology-based approach to cancer imaging. Besides research, Neel is actively involved in leadership; influencing issues pertaining to science funding, climate change, and sustainability, and outreach. He is a big admirer of cats, and looks to them for his engineering inspiration.

Neelkanth M. Bardhan

I. INTRODUCTION

In the past 30 years, there has been explosive growth in interest in the use of carbon-based nanomaterials, ever since the introduction of 0D (C60 buckminsterfullerene),1 1D (carbon nanotubes),2 and 2D (graphene)3 forms (Fig. 1) of CArbon-based NanO MATerials (CANOMATs), in that chronological order, where D refers to the dimensionality. These low-D CANOMATs are exceptionally advantageous for biomedical applications, because of their unique optoelectronic, chemical, mechanical, and physical properties and their large surface area,4–7 coupled with dimensions Contributing Editor: Adrian B. Mann a) Address all correspondence to this author. e-mail: [email protected] DOI: 10.1557/jmr.2016.449

that are comparable to those of biomolecules such as DNA or proteins.8 For a brief overview of the properties of pristine CANOMATs, the reader is referred to the Supplementary Material. What makes these materi