How Magnetic Composites are Effective Anticancer Therapeutics? A Comprehensive Review of the Literature

Figures & data

Table 1 Categories of Magnetism Materials and Their Characteristics

Type	Example, Refs	Net Magnetization	Response to EMF	Response After Removing EMF	Susceptibility
Diamagnetic	Au, Ag, and most of known elements, ^Citation51,Citation52	0	Weak response, aligned contrary to the applied EMF	Do not retention of magnetic moment	Very small and negative (−10-4 to −10-6)
Paramagnetic	Na, Mg, Al, Ga, Li, Ta, Cu,^Citation53	✓	Sectional response, aligned positive to the direction of EMF	No retention of magnetic moment	Small and positive (10–4 to 10–6)
FM	Fe, Co, Ni,^Citation54	✓	Potent response, aligned parallel to EMF	Remains a residual magnetic moment	Very large and positive (104 to 106)
Antiferromagnetic	MnO, CoO, NiO, CuCl2,^Citation55	0	Potent response, aligned parallel to EMF	A residual magnetic moment remains	Small and positive (0.1–1)
FiM	BaFe12O19 Fe3O4, MnFe2O4, Magnetite (Fe3O4) and maghemite (γ-Fe2O3),^Citation56	✓	Potent response, aligned parallel to EMF	A residual magnetic moment exists after the removal of EMF	Large and positive (103 to 105)

Figure 1 (a) Schematic of popular methods for synthesis of MNPs, (b) Representation of the principle of nanoparticle nucleation due to LaMer’s mechanism of (sulfur) nucleation.^67,68 (c) MHT using MNCs for different biomedical applications.⁷⁰

Table 2 Various Methods for Synthesis of MNPs

Routes	Methods	Condition	Temp (°C)	Duration (min/hrs/d)	Nano-Size	Capability of Morphology Control	Production Scale	Refs
Chemical	Co-precipitation	Facile in ambient conditions	20–150	Quick (min)	Small	Poor	Large	[80,81]
Chemical	Sol-gel synthesis	Difficult	25–200	Average (hrs)	Small	Good	Normal	[82,83]
Chemical	Electrochemical	Difficult	Room	Slow (hrs - d)	Small	Good	Normal	[84,85]
Green	Biosynthesis	Difficult	Room	Slow (hrs)	Average	Poor	Large	[86,87]
Green	Green-based	Easy	Room	Quick (min - hrs)	Small	Poor	Large	[20,37]
Physical	High-temperature thermal decomposition	Difficult	100–350	Slow (hrs - d)	Very small	Good	Large	[88,89]
Physical	Hydrothermal or solvothermal synthesis	Facile, High pressure	150–220	Slow (hrs - d)	Very small	Great	Large	[90,91]
Physical	Pulsed laser ablation pyrolysis	Difficult	Room	Quick (min - hrs)	Small	Good	Large	[92,93]
Physical	Microwave-assisted	Difficult	Room	Slow (hrs)	Average	Good	Normal	[94,95]
Physical	Microemulsion	Difficult	20–80	Average (hrs)	Small	Good	Small	[96,97]
Physical	Sonolysis or sonochemical	Very facile	20–50	Very quick (min)	Small	Poor	Normal	[98,99]
Physical	Aerosol/vapor	Difficult, controlled conditions	Above 100	Average (min- hrs)	Small	Good	Large	[100,101]

Table 3 Various Polysaccharides Utilized in Composites

Polysaccharide	Source	Charge	Main Functional Groups	Ref.
Cellulose	Botanical and bacteria	Negative	OH	[138]
Chitosan	Shells of crustaceans such as shrimp, lobster, crayfish and oyster	Positive	OH, COO−, NH2	[9]
Starch	Microbial product in wine, glucose, plants	Neutral	OH	[139]
Alginate	The cell wall of brown marine algae	Negative	OH, COO^−	[140]
Mannan	Plant	Neutral	OH	[141]
Hyaluronic acid	Connective, epithelial, and neural tissues	Negative	OH COOH	[142]
Heparin	Animal tissues	Negative	OH OSO3H	[143]
Pullulan	Fungus Aureobasidium pullulans	Neutral	OH	[144]
Levan	Archaea, fungi, bacteria, and a limited number of plant specie	Neutral	OH	[145]
Elsinan	Fungi, bacteria	Neutral	OH	[146]
Gellan	Bacterium Sphingomonas elodea	Negative	OH	[147]
Curdlan	Fungi, bacteria	Positive	OH, COO^−	[148]
Succinoglycan	Agrobacterium sps, Rhizobium sps, Rhizobium meliloti, Alcaligenes faecalis	Negative	OH	[149]
Zooglan	Zoogloea ramigera	Negative	OH	[150]
Xanthan	Xanthomonas campestris	Negative	OH	[151]
Dextran	Leuconostoc mesenteroides, Lactobacillus spp and Streptococcus mutans	Neutral	OH	[152]

Figure 2 Inorganic and organic materials and their properties regarding their use as functionalizing and coating agents for the synthesis of MNCs.¹⁶³

Figure 3 Different coating structures for synthesis of MNCs and common shapes of the magnetic core.¹⁷¹

Figure 4 TEM morphologies and size distribution of (A) Fe₃O₄ NPs and (B) PMNCs of Fe₃O₄@C. (C) Raman spectrum, (D) XRD, (E) FTIR spectrum (F), TGA curves, and (G) M_s of Fe₃O₄ and Fe₃O₄@C.¹³⁶

Figure 5 (a) Schematic presentation of thermal dissipation process (Néel and Brownian relaxation processes) from MNCs under AMF.^188,189 (b) The SAR value of MNPs related to (i) M_s, (ii) K, and (iii) particle size (r) with SLP, respectively.^188,189 (c) Illustration of different methods for hyperthermia treatment.¹⁹⁰

Table 4 Overview of the Recent Studies on SAR Values of MNPs, MNCs, and PMNCs with Respect to Size, Morphology, and Factors Used in Magnetic Hyperthermia Analysis

Magnetic Composites	Type of Analysis, Shape, Size (nm)	Field (kA/m)	Frequency (kHz)	SAR (W/g)	Ref.
Fe3O4/poly(styrene-co-maleic anhydride)	TEM, nanoclusters, 33	23.8	302	253	[191]
Fe3O4/PVP	TEM, spherical, 45	32.5	400	1100	[192]
Fe3O4/graphene oxide	TEM, spherical, 45	32.5	400	5160	[192]
CoFe2O4	TEM, spherical, ~ 10	30.1	265	91.84	[193]
Ag-Fe3O4	TEM, spherical, ~ 10	13.9	274	43	[194]
NiFe2O4	TEM, spherical, 4.4	23.7	170	~ 11	[195]
Fe3O4/PEG	TEM, cubes, 19	29	520	2452	[196]
CoFe2O4	TEM, spherical, 5.4	95.6	329	~76	[197]
Co0.03Mn0.28Fe2.7O4/SiO2	TEM, spherical, ~22	33	380	~3417	[198]
Fe3O4/citric acid	TEM, spherical, ~10	35.88	316	49	[199]
Fe3O4/PEG	TEM, spherical, ~10	35.88	316	56	[199]
Fe3O4/ethylene diamine	TEM, spherical, ~10	35.88	316	77	[199]
Fe3O4/cetyl-trimethyl ammonium bromide	TEM, Spherical, ~10	35.88	316	47	[199]
Fe3O4/citric acid/PEG	TEM, spherical, ~10	35.88	316	60	[199]
Zn0.5Ca0.5Fe2O4	TEM, spherical, 12–14	10.2	354	~14.8	[200]
Zn0.33Fe2.67O4	TEM, spherical, ~8	35.7	360	~178	[201]
Gd-doped Mg-Zn ferrites	TEM, spherical, 50–200	5.0	600	~15–27.5	[202]
Fe3O4/garcinia mangostana fruit peel extract	TEM, spherical, ~13	75	318	98	[20]
		100	313	130
		125	312	179
Fe3O4/Punica Granatum fruit peel extract	TEM, spherical, ~11	75	318	196	[203]
		100	313	212
		125	312	232
Fe3O4	Nr	0.450	400	46.8	[204]
Fe3O4@agar	TEM, spherical, 9.2	0.450	400	23.6	[204]
Chitosan/trimethylammonium/ SPION	TEM, spherical, 13.7	27.57	360	168	[205]
Chitosan/curcumin/alginate/SPION	Nr	27.57	360	280	[205]
Peptide nucleic acid oligomers/SPION	TEM, spherical, ~15	17	183	65	[206]
CoFe2O4/meso-2,3-dimercaptosuccinic acid/DOX	TEM, spherical, 13	30	307	94.58	[207]
Chitosan/Fe3O4/5FU	SEM, spherical, 125	35	180	Nr	[208]
Fe3−δO4@silane and a thermoresponsive copolymer shell composed of 2-(2-methoxy)ethyl methacrylate and oligo(ethylene glycol)methacrylate moieties (1.14 mL)	TEM, spherical, 10	23.8	536.5	25.2	[209]
Fe3-δO4@silane and a thermoresponsive copolymer shell composed of 2-(2-methoxy)ethyl methacrylate and oligo(ethylene glycol)methacrylate moieties	Dynamic light scattering (DLS), Not reported (Nr), 55–80	23.8	536.5	61.7	[209]
Fe3-δO4@silane	DLS, Nr, 20–30	23.8	536.5	100	[209]
Graphene quantum dots-Fe3O4/SiO2	TEM, Nr, 100	14.3	409	44	[210]
DOX loaded Fe3O4/MamC/proteinAR-3 mAbs (IgG1)	TEM, Nr, 36	12.5	273	53	[211]
			205	41
			163	22
			143	19
Magnetite	TEM, spherical, 30	12.5	273	68	[211]
			205	47
			163	28
			143	24
Alginate-chitosan-Fe3O4	Nr	40	265	720	[212]
CuFe2O4	TEM, spherical, 17.3	28.5	126	192	[213]
		25.7	126	185.2
		22.2	126	177.8
		18.6	126	171.5
CuFe2O4	TEM, spherical, ~19.9	19	120	44.9	[91]
		16	120	38.0
		13	120	24.8
CuFe2O4	TEM, spherical, ~25	13.5	331	6.48	[95]
Mn0.5Zn0.5Fe2O4	TEM, spherical, ~14	6.37	178	28.38	[214]
MgFe2O4	TEM, spherical, ~9	9.2	198	~19	[215]
Solvent optimized redox tuned iron oxide	TEM, spherical, ~25	50	100	~700	[216]
Thermosensitive polymer poly(2-(dimethylamino)ethyl methacrylate) coated Fe3O4	SEM, irregular–quasi-spherical, 98	16.15	205	150	[217]
Fe3O4/hexadecylamine/oleic acid/1-octanol	TEM, rods, ~56 (length) × 10 (width)	63.81	310	862	[218]
Graphene oxide-Fe3O4-PEG	TEM, spherical, ~20	12.57	293	557.38	[219]
PLGA/Fe3O4/DOX/PVA	TEM, spherical, 172	2	205	36.27	[220]
PLGA/Fe3O4	Nr	2	205	35.73	[220]
Cetyltrimethylammonium bromide@Fe3O4	TEM, cubic, ~ 80	63.66	315	1036	[221]
Fe3O4	TEM, Pseudo spherical, 12.97	15.9	252	63.4	[222]
Fe3O4@citric acid	DLS, 46.9	15.9	252	65.8	[222]
Fe3O4@(3-aminopropyl)triethoxysilane	DLS, 68.1	15.9	252	67.2	[222]
Fe3O4@dextran	DLS, 76.6	15.9	252	55.6	[222]
SPIONs coated with PEG4.9kD-PLA6.0kD	TEM, Cubic, 18	59.6	346	558	[223]
IONPs	TEM, Cubic, 30–35	63.3	310	800	[224]
Chitosan coated Fe3O4	TEM, spherical, 37	14	335	595	[84]
Fe3O4	TEM, cubic, 37	23.9	571	213	[98]
mSiO2@Fe3O4	TEM, spherical, ~100	22	120	13.84	[89]
Poly(Nisopropyl acrylamide-co-acrylic acid)@mSiO2@Fe3O4	TEM, spherical, ~100	22	120	8.22	[89]
Fluorescent IONPs/PLGA conjugated with human epidermal growth factor receptor 2	DLS, Nr, 524	16.27	440	183	[225]
IONPs - (poly(maleic anhydride-alt-1-octadecene)- (tetramethylrhodamine 5(6)-carboxamide cadaverine - N-(3 dimethylaminopropyl)-N′-ethylcarbodiimide hydrochloride - 4-aminophenyl β-D glucopyranoside	TEM, spherical, 11.3	20	829	104	[226]
PEG coated SPIONs	TEM, spherical versus cubic, 33	9.35	300	1010	[227]
PEG coated SPIONs	TEM, spherical versus cubic, 40	20.7	300	1026	[227]
Chitosan coated Fe3O4	TEM, spherical, 30–40	20	335	711	[228]
Graphene oxide-Fe3O4	TEM, spherical, 10–21	16.72	325	543	[85]
Silica coated lanthanum strontium manganese oxide	TEM, irregular, 35	13	335	295	[229]
Chitosan-g-N-isopropylacrylamide coated Fe3O4-silica	TEM, spherical, 30–50	3	100	9.75	[230]
Fe3O4	TEM, spherical, 5–10	3	100	15.80	[230]
Trimesic acid coated SPIONs dispersed in triethylene glycol	TEM, spherical, 9	10.9	751.5	276.3	[231]
		13.8	262.2	81.2
Tetraethyl orthosilicate coated La0.7Sr0.3MnO3	TEM, wormhole-like mesopores, 45	14	350	255	[232]
Citric acid coated HoxFe3xO4	TEM, spherical, 10–15	23.87	488	337.3	[233]
Pluronic F127 coated Mn0.6Ga0.4Fe2O4	Nr	10.18	354	160.9	[234]
Cetyltrimethylammonium bromide and polycaprolactone coated Fe3O4	TEM, spherical, 21	15.75	312	255.12	[235]
Aminosilane coated Fe3O4	DLS, Nr, 100	23.87	557	320	[161]
Dextran coated Fe3O4	TEM, irregular, 21	11.93	150	52.3	[154]
Polyphenol coated Fe3O4-γFe2O3	TEM, spherical, 10–14	23.87	570	Nr	[236]
Fe3O4	TEM, spherical, 27	Nr	13,560	725	[237]
Citric acid coated MnxFe3-xO4	TEM, spherical, 34	13.36	405	Nr	[160]
Stevioside coated Fe3O4	TEM, spherical, 3	13.36	405	80	[159]
Oleic acid coated Fe3O4	TEM, Nr, 45	26.67	265	80	[162]
Chitosan coated MnFe2O4	TEM, cubic, 18	60	307	270	[153]
PEG NiFe2O4	TEM, rod, 16	3.89–5.49	260	17–22	[155]
Phosphate coated Fe3O4	TEM, spherical, 14	0.819	126	11.1	[156]
Tetraethyl orthosilicate coated MnFe2O4	TEM, spherical, 14	5.49	260	47.8–84.65	[157]
Zn0.9Fe0.1Fe2O4	TEM, spherical, 11	2.73	700	36	[158]

Table 5 Overview of Some Recent in vitro Studies on MNCs for MHT and Targeted Drug Delivery Systems

Magnetic Nanoagent	Type of Analysis, Size (nm)	Loaded Drug	Drug Release	Origin, Type, Cell Lines	Results	Ref.
Monoclonal antibody conjugated Fe3O4	TEM, 36	DOX	~60% release at pH 5.0 medium with AMF	Gastric, cancer, GTL-16	Chemotherapy and combined therapy caused 20% and 78% cancer cell death, respectively	[261]
Silica-Fe3O4	TEM, ~ 30	Maytansinoid	Nr	Macrophage, cancer, IC21	Chemotherapy, MHT, and combined therapy caused 20%, 15%, and 78% cancer cell death, respectively	[262]
Oleosome-ZnFe2O4	TEM, ~80	Carmustine	~4% and ~23% release at pH 7.2 medium without and with AMF, respectively	Breast, cancer, SK-BR-3	Chemotherapy, MHT, and combined therapy caused 60%, 40%, and 80% cancer cell death, respectively	[263]
Fe3O4@agar	TEM, 9.2	DOX	85% release at pH 7.0 medium	Colon, cancer, HT-29	Combined therapy caused ~85% cancer cell death	[204]
MnFe2O4/ω-hydroxyacid-co-poly(d,l-lactic acid)	DLS, 160	Paclitaxel	~98% release within 18 days at 7.4 medium	Colon, cancer, Caco-2 and hASCs	The elimination of cancer cell was dose-dependent and significantly increased after treatment with increasing sample concentration (1000 µg/mL)	[264]
Malic acid/Fe3O4	TEM, 9.2	DOX	~79% release at pH 6.5 medium. ~22% release at pH 7.4 medium	Breast, cancer, MCF-7	65% cancer cell death without AMF	[265]
Magnetic nano/micro‑particles based on clinoptilolite‑type of natural zeolite	SEM, 75	Nr	Nr	Nr	The temperature in the MCZ injected chicken wing is increased from 27.5 °C to 32.1 °C in 5 min and to 39.7 °C in 22 min with AMF	[266]
Mn0.5Zn0.5Fe2O4@PEG nanofluid	TEM, 6.5	Nr	Nr	Retinal, cancer, ganglion	Controlling the recovery time during MHT affects the cell death rate	[267]
CuFe2O4	TEM, 17.3	Nr	Nr	Colon, cancer, HT-29	53% cancer cell death without AMF	[213]
Graphene oxide/ CoFe2O4	TEM, 5	Nr	Nr	Breast, cancer, MCF-7	42% and 70% cancer cell death without and with AMF, respectively	[268]
PVA-Mg-Co-Fe2O4	DLS, <120	5FU	Nr	Breast, cancer, MCF-7 and cervical, cancer, HeLa	>65% cancer cell death without AMF	[269]
Chitosan/Fe3O4	SEM, 125	5FU	45% release at pH 7.4 medium	Glioblastoma, cancer, A-172	25% cancer cell death with AMF and no significant elimination of normal cells fibroblasts	[207]
Fe3−δO4@silane and a thermoresponsive copolymer shell composed of 2-(2-methoxy)ethyl methacrylate and oligo(ethylene glycol)methacrylate moieties (1.14 mL)	TEM, 10	DOX	100% release after 52-hr at 42 °C and pH 7.4 medium. 62% release after 52-hr at 37 °C and pH 7.4 medium	Ovary, cancer, SKOV-3	~70% cancer cell death at 41 °C	[209]
Fe3−δO4@silane and a thermoresponsive copolymer shell composed of 2-(2-methoxy)ethyl methacrylate and oligo(ethylene glycol)methacrylate moieties (1 mL)	DLS, 55–80	DOX	100% release after 52-hr at 42 °C and pH 7.4 medium. 70% release after 52-hr at 37 °C and pH 7.4 medium	Nr	Nr	[209]
Graphene quantum dots/Fe3O4/SiO2	Nr	DOX	30% and 45% release at pH 5.0 medium with 37 °C and 50 °C, respectively	Breast, cancer, 4T1	18%, 80%, and 92% cancer cell death without, with AMF one, and two times, respectively. Chemotherapy, MHT, and combined therapy caused 40%, 65%, and 80% cancer cell death, respectively	[210]
Graphene quantum dots/Fe3O4/SiO2	TEM, 100	Nr	Nr	Breast, cancer, 4T1	44% and 52% cancer cell death without and with AMF, respectively.	[210]
Fe3O4/MamC/proteinAR-3 mAbs (IgG1)	TEM, 36	DOX	44% and 25% release at pH 7.4 medium with and without AMF. 6% and 2% at pH 5.0 medium with and without AMF	Colorectal, cancer, HT-29	7% and 18% cancer cell death without and with AMF, respectively	[211]
La0.7Sr0.3MnO3/PEG	TEM, 15–20	DOX	46% and 14% release at pH 5 and 7.4 medium without AMF, respectively	Breast, cancer, MCF-7	29% and 90% cancer cell death without and with AMF, respectively	[270]
Human serum protein/La0.7Sr0.3MnO3/PEG	Nr	DOX	39% and 12% release at pH 5 and 7.4 medium without AMF, respectively	Breast, cancer, MCF-7	16% and 79% cancer cell death without and with AMF, respectively	[270]
Alginate-chitosan-Fe3O4	TEM, ~14	DOX	22.5% and 0.2% release in tumor site with and without AMF, respectively	Breast, MCF-7	Chemotherapy, MHT, and combined therapy caused 85%, 63%, and 95% cancer cell death, respectively	[212]
ZIF-90 on polydopamine-coated Fe3O4	SEM, 200	DOX	17.3%, 70.8%, and 88.7% release at pH 7.4, 6.0, and 4.5 medium after 24 h, respectively	Cervical, cancer, HeLa	Chemotherapy, MHT, and combined therapy caused 32%, 50%, and 72% cancer cell death, respectively	[271]
Ferumoxytol-medical chitosan	Nr	DOX	~100% drug release at 43 °C and pH 5.2 medium	Colon, cancer, HT-29	Chemotherapy, MHT, and combined therapy caused 32%, 50%, and 72% cancer cell death, respectively	[272]
Lipid based Fe3O4	TEM, ~50	Temozolomide	61.3% and 100% at pH 7.4 and 4.5 medium after 7 days with AMF	Glioma, cancer, Uppsala 87	Chemotherapy, MHT, and combined therapy caused 10%, 44%, and 50% cancer cell death, respectively.	[273]
IONPs stabilized with trimethoxysilylpropyl-ethylenediamine triacetic acid as a carrier of DOX	TEM, 4.76	DOX	40% and 65% release within 2-hr at pH 7 and 5 medium, respectively	Mouse brain-derived microvessel endothelial, bEnd.3, Madin–Darby canine kidney transfected with multi-drug resistant protein 1 (MDCK-MDR1), and human U251 GBM cells	The combination of magnetic enhanced convective diffusion and the cadherin binding peptide for transiently opening the blood–brain barrier tight junctions are expected to enhance the efficacy of cell death (over 90%) within 48-hr of treatment using the DOX-EDT-IONPs	[274]
PEG coated NiFe2O4	TEM, 55	DOX	Release rate of 1.33% per min.	Nr	Nr	[275]
IONPs/PLGA fiber	TEM, 600 nm fiber and 20 nm IONPs	Bortezomib	18% and 70% release at 7.4 and 5.5 medium.	Fibroblast, cancer, NIH3T3 and mouse mammary carcinoma, 4T1	Many of the cells exhibited a shrunken morphology with membrane blebbing on their surface	[276]
Lectrospun chitosan/cobalt ferrite/titanium oxide nanofibers	SEM, 110	DOX	~85% and ~52% release at 5.3 and 7.4 medium with AMF. ~63% and ~40% release at 5.3 and 7.4 medium without AMF	Melanoma, cancer, B16F10	78% cancer cell death with AMF	[277]
Graphene Oxide-Fe3O4-PEG	TEM, ~20	DOX	~58% and ~19% release at 5 and 7.4 medium without AMF	Murine, cancer, colorectal, CT26	80% cancer cell death with AMF	[219]
PLGA/Fe3O4	TEM, 172.1	DOX	Nr	Colon, cancer, CT26	~80% cancer cell death with AMF	[220]
Mg0.13-Fe2O3	TEM, 7	Nr	Nr	Glioblastoma, cancer, U87MG	75% and 100% cancer cells death at a temperature of 48.4 °C and 63.5 °C with AMF, respectively	[278]
Ether triad modified core-shell magnetic mesoporous silica	TEM, 50–60	DOX	55.3%, 73.5%, and 85% release at pH 6.5, 5.0, and 4.0 medium, respectively, after 24-hr without AMF. 3.6%, 4.5% and 6.2% release at 25 °C, 37 °C, and 45 °C in pH 7.4 medium without AMF. 80%, 88%, and ~ 95% release at 25 °C, 37 °C, and 45 °C, respectively, at pH 7.4 medium with AMF.	Breast, cancer, MDA-MB-231	~5% and 77% cancer cell death without and with AMF, respectively	[279]
Fe3O4@PLA-grafted P (HEMA-co-MAA-co-NIPAAm-coTMSPM)	SEM, 96	DOX, Methotrexate	40% MTX and 75% DOX release at 41 °C in pH 4 medium after 6 days	Nr	Nr	[280]
Poly(Nisopropyl acrylamide-co-acrylic acid)-co-AAc)@mSiO2@Fe3O4	TEM, ~100	5FU	7.8% and 47% release after 20-hr with AMF at 37 °C and 45 °C, respectively	Nr	Nr	[89]
IONPs - (poly(maleic anhydride-alt-1-octadecene)- (tetramethylrhodamine 5(6)-carboxamide cadaverine - N-(3 dimethylaminopropyl)-N′-ethylcarbodiimide hydrochloride - 4-aminophenyl β-D glucopyranoside	TEM, ~11	Nr	Nr	3D pancreatic, cancer tumor, MIA PaCa-2	72% cancer cell death with AMF	[226]
Chitosan coated Fe3O4	TEM, 30–40	Nr	Nr	Lung, cancer, A549	50–70% cancer cell death with AMF	[228]
Graphene oxide - Fe3O4	TEM, 10–21	Nr	Nr	Lung, cancer, A549	80.5% cancer cell death with AMF	[85]
Silica coated lanthanum strontium manganese oxide	TEM, 35	Nr	Nr	Lung, cancer, A549	~75% cancer cell death without AMF	[229]
Chitosan-g-N-isopropylacrylamide coated magnetic-silica	TEM, 30–50	DOX	83.30% release after 5-hr with AMF at 45 °C and pH 4.0	Neck, cancer, Cervical	90.83% cancer cell death with AMF	[230]
Trimesic acid coated SPIONs dispersed in triethylene glycol	TEM, 9	Nr	Nr	Breast, cancer, MCF-7	90% cancer cell death with AMF	[231]
Tetraethyl orthosilicate coated La0.7Sr0.3MnO3	TEM, 45	Nr	Nr	Lung, cancer, A549	80% cancer cell death with AMF	[232]
Cetyltrimethylammonium bromide and polycaprolactone coated Fe3O4	TEM, 21	Nr	Nr	Liver, cancer, HepG2	~60% cancer cell death with AMF	[235]
CoFe2O4	TEM, ~10	Nr	Nr	Mouse fibroblast, normal, L929	15% normal cell death without AMF, showing high biocompatibility	[193]
Oleic acid/PEG coated CoFe2O4	TEM, ~10	Nr	Nr	Mouse fibroblast, normal, L929	0% normal cell death with AMF, showing high biocompatibility	[193]
Co0.03Mn0.28Fe2.7O4/SiO2	TEM, ~22	Nr	Nr	Osteosarcoma, normal, MG-63 and MEF	Less than 3% normal cell death without AMF, showing high biocompatibility	[198]
Contractible hydroxypropyl methyl cellulose/Fe3O4 hydrogel	TEM, 200	DOX	57.6% and 32.3% release with and without AMF in 24-hr at pH 7.4 medium. 78.8% and 41.7% with and without AMF at pH 5.5 medium	4T1 breast cancer	No tumor recurrences occurred in the chemo-thermal therapy group after 21 days of MHT	[207]
Fe3O4 NPs-silica-poly(Nisopropyl acrylamide-co-acrylic acid)	Nr	5FU	7.8% and 47% release after 20-hr at 37 °C and 45 °C, respectively	Nr	Nr	[89]
IONPs coated with graphite-like shell and labeled with Alexa 647 fluorescent marker	Nr	Nr	Nr	Nr	With an applied field of 38 kA/m at 980 kHz, tumors could be heated to 60 °C in 2 minutes, durably ablating them with millimeter (mm) precision, leaving surrounding tissue intact	[281]

Figure 6 TEM images of (a) SPIONs, (b) SPION@CA, (c) SPION@CA-Dox, and (d) SPION@CA-epirubicin.²³³ (e) TEM image and the particle size distribution analysis of DOX-Fe₃O₄@agar, (f) Magnetic strength of Fe₃O₄ and DOX-Fe₃O₄@agar, (g) Drug release profiles of DOX-Fe₃O₄@agar at pH 7, (h) The SAR values and temperature achieved by Fe₃O₄, DOX-Fe₃O₄@agar, and DOX-Fe₃O₄@agar in HT-29 cells under applied AMF (applied field = 400 A, frequency = 250 kHz), (i) Schematic of effects of DOX-Fe₃O₄@agar for eliminating HT-29 cancer cells under hyperthermia, (j) fluorescence microscopy images of HT-29 cells after 1-hr of incubation with DOX-Fe₃O₄@agar, and (k) Cell survival of HT-29 cells treated by DOX-Fe₃O₄@agar with and without MHT.

Notes: The significance levels denote as * (p < 0.05), ** (p < 0.01), and *** (p < 0.001) indicate the degree of statistical significance when compared to the control group. (i, j, and k) Reprinted from Wang Y-J, Lin P-Y, Hsieh S-L, et al. Utilizing edible agar as a carrier for dual functional doxorubicin-Fe3O4 nanotherapy drugs. Materials. 2021;14(8):1824. Creative Commons.²⁰⁴

Table 6 The in vivo Studies on MNCs for MHT and Targeted Drug Delivery

Magnetic Nanoagent	Type of Analysis, Size (nm)	Loaded Drug	Drug Release	Cell Lines	NP Administration Route, Animal Model	Results	Ref.
PLGA/Fe3O4	TEM, 172	DOX	Nr	CT26 colon cancer in 5 mice	Intratumoral injection, Mouse	The tumor size decreased 4 times with AMF	[220]
Commercially available “biocompatible” type of MNPs	TEM, 15	Nr	Nr	Nr	Injected intravenously via a tail vein, Mouse	By direct intratumoral injection of MNPs, tumor size decreased 60% in 14 days (amount of Fe ∼17 mg). In addition, 5 out of 5 mice were tumor free at 120 days. They had an initial tumor size of 1.5 cm (amount of Fe ∼6 mg + injections for retreatment).	[282]
Commercially available “biocompatible” type of MNPs	TEM, 11	Nr	Nr	OVCAR-3 ovarian tumor cells	Injected intravenously via a tail vein, Mouse	7 out of 9 (78%) tumor free after 160 days	[282]
Fluorescent IONPs/PLGA conjugated with human epidermal growth factor receptor 2	DLS, 524	Gemcitabine	23% release in 5 minutes at 440 kHz frequency (16.27 kA/m) and sustained drug release for 11 days	MIAPaCa-2 in SCID mice	Intravenous injection, Mouse	The tumor regression study at the end of 30 days showed significant tumor regression (86±3%) with MHT	[225]
Mg0.13-Fe2O3	TEM, 7	Nr	Nr	Hep3B xenografted animal models	Injected into the tumor directly, Mouse	It was clearly observed that the tumor was completely killed after 2 days with AMF.	[278]
Fe3O4/Poly(ethylene glycol) methyl ether	SEM, 73	Nr	Nr	Nude mice xenografted with breast cancer MCF-7	Injected into the tumor directly, Mouse	Following treatment, the tumor volumes were monitored for up to 40 days. For the control mice, tumor size increased 25 fold by the fortieth day. With AMF (1.2 × 109 A m^−1 s^−1), from the sixth day onwards, tumors were completely eliminated without recurrence within the experimental period	[283]
Biomimetic magnetic NPs mediated by magnetosome proteins	TEM, 36	DOX	100, 300, and 500 µg of BMNPs were exposed at (130 kHz and 18 kA m^−1) for 20 min	4T1 and MCF-7 in Balb/c female mice of about six weeks old	Tail-vein injection, Mouse	Around 40% of the tumor size decreased by MHT and chemotherapy, which was higher than chemotherapy alone.	[284]
Graphene oxide-cobalt ferrite	TEM, 5	Nr	Nr	MCF7	Injected in situ to the multiple points of the tumor, Mouse	BALB/c mice and the results indicated the smaller size of the tumor with the concentrations of 0.001 and 0.002 gr/mL and the respective magnetic frequencies of 400 and 250 kHz for 10 min after 27 days	[268]
IONPs-(poly(maleic anhydride-alt-1-octadecene)- (tetramethylrhodamine 5(6)-carboxamide cadaverine-N-(3 dimethylaminopropyl)-N′-ethylcarbodiimide hydrochloride-4-aminophenyl β-D glucopyranoside	TEM, ~11 DLS, ~85	Nr	Nr	Pancreatic tumor cell line (MIA PaCa-2)	Intratumoral injection, Rat tail	∼47% and ∼14% antitumor effects in heterotopic xenograft mouse model with and without AMF, respectively.	[226]

Figure 7 (a) Interaction of BMNPs with 4T1 cells in the presence/absence of a continuous gradient magnetic field analyzed at TEM, micrographs of the cells incubated with the 100 µg/mL of BMNPs for different periods of time. The micrographs are representative of alternate serial cuts of the cell pellets of each sample. Scale bar, 5 µm. (b) In vivo antitumor activity of BMNPs under the influence of AMF, Images were captured using a thermic camera of a representative mouse without (left) and with (right) injected BMNPs during AMF treatment. Note the different colors within the circle on the backside of the mouse.²⁸⁴

Figure 8 (a) Schematic of pH, magneto, and thermo-responsive drug delivery systems using drug-loaded MNCs. (b) The schematic of prospective use of drug-loaded MNCs for hyperthermia and magnetic targeted cancer therapy.^220,318

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