Revealing the Toxicity of Chlorate through the Analysis of Molecular Interaction Using Viscosity Measurements and Apparent Molar Volumes

Introduction

Lychees and longans are close family members. longans and lychees are comparable in nutritional composition. Both are minimal in calories and carbohydrates and are nil in fat. The antioxidants and fibres are abundant in longan and lychee similarly are great source of vitamin C .

Figure 1: Lychee Fruit Click here to View figure

Figure 2: Longan Fruit. Click here to View figure

Longan (Dimocarpus longan), a subtropical fruit plant belonging to the Sapindaceae family, is ideally suited to tropical regions with distinct wet/dry seasons as well as subtropical locales with a cool, nonfreezing fall/winter period. In India, it is one of the minor fruits. There is currently insufficient documentation on longan production in India to analyze the real scenario. The longan is an important crop in Southeast Asia economically. Although leaves and flowers are sold in markets, they are not used in traditional medicine. The dried flowers are shipped to Malaysia to be used as medicine.

Off-season flowering and fruit production is a desirable economic and scientific goal for many subtropical fruit plants. The discovery of potassium chlorate to induce off-season flowering in longan, as well as off-season longan production methods in Thailand, including soil drench (Manochai S. W.-a., 1999) ( (Sritontip C. Y., 1999)), foliar spray ( (Sritontip C. Y., 1999)), and truck or stem injection ( (Viriya-alongkorn, 1999)).

Though chlorate is able to precisely induce flowering in longan, it also causes toxic effects on the crop. KClO₃ serves as a herbicide or a defoliant on many other plants. (Nahar, 2010) (Manochai P. J., August 2008)

While chlorate is able to specifically induce flowering in longan, it also causes toxic effects on the crop. (Sritontip C. Y., 2003).Great concern is paid upon the toxicity of chlorate (Daniel, 1990) because  of heavy introduction of this chemical into the environment from paper making industry. (Moore & Calabrese , 1982). An increasing demand from end user industries, such as farming, explosives, laboratories and disinfectants is predicted to contribute significantly to the growth of the potassium chlorate market in the forecast timeframe. The explosives based on potassium chlorate are more effective than ordinary powder. The production of fireworks and matching bands also involves extensively utilised potassium chlorate. In smoke compositions such as smoke grenades it is utilised as a component. In laboratories and educational facilities, potassium chlorate is used to generate oxygen, other than explosives. It is also utilised for the destruction of pests as a pesticide in agriculture.  (https://www.businesswire.com/portal/site/home/my-business-wire/, 2020)

A significant amount of information is needed on the properties of transport, thermodynamic and solution to comprehend how the co-solvent or co-solute can change the nature and structure of the water. (Bahadur, 2019)

This work examines the interaction like ion-solvent, ion-ion and solvent-solvent of potassium chlorate with aqueous ionic salts, as both the solute and solvents are utilised for agricultural operations.

In this study the chemical and the electrostatic effect due to dielectric constant of the co-solute which are already present in soil like KCl, KNO₃ and NH₄NO_{3 ,} KH₂PO₄ would play vital role in influencing solute-solvent interaction. (Ganjare, 2020). Viscosity data can be used to determine the diffusion controlled reaction rate constant kd.

The current study used multi-component systems containing an ionic solid, water, and KClO₃ (ionic solids = KCl, KNO₃, and NH₄NO_3, KH₂PO₄))to evaluate the relationship between the transport properties of KClO₃ solutions in aqueous electrolyte solutions and solution concentrations and temperature.

The densities of aqueous solutions were measured using 15cm³ double arm pycnometer in a transparent glass walled water bath. (Kharat, 2007) Triple distilled water was used to calibrate the pycnometer. At desired temperatures, the densities of KClO₃ solutions in aqueous 1 % KCl, KNO₃ and NHNO_{3 ,}  KH₂PO_4, and pure water were determined using a bi-capillary pycnometer. An average of triplicate measurements was the final result and the density was calculated with an accuracy of ±1.25 ×10^-4 g.cm-³. The thermostat temperature is maintained at the appropriate temperatures using a demerstat with an accuracy of ±0.1 K.

Viscosities of all salt solutions of ten different concentrations in water were measured using Ubbelohde viscometer at temperatures of 298.15, 303.15, 308.15, and 313.15K. Measurements to monitor reproductibility of results have been repeated at least three times The overall precision of viscosity measurements was ± 2.0×10_–⁴ mPa.s. At 0.01 second intervals the flow time is accurately recorded.

All chemicals were taken from Sigma Aldrich, Germany, with more than 99% purity and was further desiccated over anhydrous CaCl₂­ before use. (Nanda, Nanda, & Mohanty, 2012). The sample specification is given in Table 1.

Table 1: Specification of Chemicals

Chemicals	Source	Mass fraction Purity	Purification Method	CAS No.	Mol. Mass g.Mol-1	Chemical Formula
Potassium Chlorate	Sigma Aldrich	≥99.0%	desiccated over anhydrous CaCl2­	3811-04-9	122.55	KClO3
Potassium Nitrate	Sigma Aldrich	ACS reagent, ≥99.0%	Usedas obtained	7757-79-1	101.10	KNO3
Potassium Chloride	Sigma Aldrich	≥99.0%	Used as obtained	7447-40-7	74.55	KCl
Ammonium Nitrate	Sigma Aldrich	ACS reagent, ≥98%	Usedas obtained	6484-52-2	80.04	NH4NO3
Potassium phosphate monobasic	Sigma Aldrich	≥98.0%	Used as obtained	7778-77-0	136.1	KH₂PO₄,

 

It is known the properties like density, viscosity, etc., are influenced by the presence of  oxygen atom in a molecule. The presence of such groups increases the hydrophilicity and electrostriction between water and solute particles. (Nanda, Nanda, & Dalai, 2021)

Data Evaluation

The apparent molar volumes ∅_V, were obtained from the density results using the following equation (Cui, et al., 2020) (Langore, Nikumbh, Patil, & Gaikwad, 2019)

where M is the molar mass of the KClO₃ in g mol−1, C is the concentration (mol.L^-1), P and P₀ and the densities of the solution and the solvent, respectively in g cm⁻³

The apparent molar volumes (∅_V) were plotted against the square root of concentration (C^½) in accordance with the Masson’s equation. Partial molar volumes at infinite dilution were obtained by least-squares fitting to the equation: (Caro, 2020)

Where ∅_V⁰ is the limiting apparent molar volume and S_v a semi-empirical parameter which depends on the nature of solute, solvent as well as temperature.

Table 2: Densities and Apparent molar volumes of KClO₃ solution in 1% KNO₃and distilled water at different temperatures.

Molar Conc. (C) mol/dm3	KClO3 in   1% KCl	KClO3 in 1% NH4NO3	KClO3 in   1% KNO3	KClO3 in   1%  KH2PO4	KClO3in   1% KCl	KClO3 in 1% NH4NO3	KClO3 in   1% KNO3	KClO3 in   1% KH2PO4
Density, (P )  (g.cm-3 )298.15K					Apparent molar volumes, (∅V) cm3.mol-1
0.0055	1.00376	1.00578	1.00766	1.01016	121.43	121.25	121.11	120.91
0.0085	1.00462	1.00632	1.0085	1.01173	121.34	121.1	120.9	120.71
0.0125	1.0055	1.00718	1.00954	1.01304	121.2	120.93	120.69	120.51
0.0175	1.0066	1.00889	1.0111	1.01459	121.09	120.76	120.45	120.15
0.0235	1.0079	1.01026	1.01246	1.01626	120.92	120.59	120.29	119.93
0.0305	1.00945	1.01162	1.01395	1.01845	120.82	120.4	120.1	119.76
0.0385	1.0111	1.0135	1.01623	1.02043	120.65	120.23	119.84	119.54
0.0475	1.0129	1.0158	1.01825	1.02297	120.45	120.11	119.72	119.32
0.0555	1.0144	1.0176	1.0201	1.02519	120.32	120	119.58	119.18
303.15K
0.0055	1.00318	1.00421	1.00615	1.00856	121.61	121.45	121.33	121.12
0.0085	1.00384	1.00485	1.00692	1.00931	121.52	121.32	121.12	120.92
0.0125	1.00491	1.00589	1.00807	1.01044	121.37	121.14	120.91	120.72
0.0175	1.00597	1.00695	1.00913	1.01159	121.25	120.96	120.67	120.36
0.0235	1.00706	1.00817	1.01069	1.01356	121.11	120.78	120.51	120.14
0.0305	1.00837	1.00992	1.01231	1.01535	121	120.61	120.32	119.97
0.0385	1.00995	1.01157	1.0142	1.01743	120.8	120.43	120.06	119.75
0.0475	1.0118	1.01324	1.01621	1.01957	120.65	120.32	119.94	119.53
0.0555	1.0136	1.01516	1.01812	1.02159	120.51	120.22	119.8	119.39
308.15K
0.0055	1.00268	1.00381	1.00515	1.00784	121.76	121.59	121.45	121.28
0.0085	1.00325	1.00456	1.00639	1.00871	121.64	121.47	121.25	121.07
0.0125	1.00393	1.00558	1.00708	1.00994	121.53	121.3	121.02	120.85
0.0175	1.00486	1.00646	1.00853	1.01119	121.41	121.11	120.78	120.53
0.0235	1.00613	1.00762	1.00989	1.01276	121.28	120.91	120.64	120.32
0.0305	1.00738	1.00912	1.01161	1.01475	121.15	120.76	120.43	120.15
0.0385	1.00866	1.01117	1.0134	1.01693	120.93	120.57	120.16	119.9
0.0475	1.01045	1.01304	1.01581	1.01885	120.81	120.46	120.03	119.67
0.0555	1.01185	1.01436	1.01752	1.02081	120.67	120.38	119.94	119.56
313.15K
0.0055	1.00196	1.00329	1.00475	1.00726	121.92	121.75	121.64	121.53
0.0085	1.00265	1.00406	1.00589	1.00818	121.82	121.63	121.47	121.32
0.0125	1.00326	1.00518	1.00666	1.00932	121.69	121.46	121.24	121.1
0.0175	1.00419	1.00597	1.00808	1.01079	121.57	121.27	121.01	120.78
0.0235	1.00543	1.00712	1.00916	1.01216	121.43	121.07	120.83	120.57
0.0305	1.00658	1.00872	1.01111	1.01405	121.29	120.92	120.66	120.4
0.0385	1.00814	1.01017	1.01294	1.01624	121.16	120.73	120.41	120.15
0.0475	1.00988	1.01224	1.01521	1.01835	120.97	120.62	120.26	119.92
0.0555	1.01105	1.01376	1.01687	1.02014	120.87	120.54	120.19	119.81

The apparent molar volumes of transfer at infinite dilutions ∆ фv ⁰ (tr) of KClO₃ obtained from the relation.

The positive ∆ ∅_V⁰ (tr) studied in the present investigation suggest that the ion-ion and ion-hydrophilic group interactions are stronger than the ion hydrophobic interaction that results in an increase in volume.

The viscosity results for the aqueous solutions of KClO₃ in aqueous solute systems and pure water solvent systems were plotted in accordance with Jones-Dole equation (Lomesh , Nathan, Bala , & Thakur, 2019)

ηr-𝟷 /C½ = A + BC½                                                          (3)

Where η_r = (η/η_o) and η, η_o are viscosities of the solution and solvent respectively, C is the molar concentration.

Table 3

Molar Conc. (C) mol/dm3	KClO3 in 1% KCl	KClO3  in 1% NH4NO3	KClO3 in 1% KNO3	KClO3 in 1% KH2PO4	KClO3  in  1% KCl	KClO3  in 1% NH4NO3	KClO3 in  1% KNO3		KClO3 in  1% KH2PO4
	Viscosities (η) (Nm-3.s) 298.15K				Relative viscosities (ηr) 298.15K
0.0055	0.9296	0.9324	0.9359	0.9439	1.0358	1.0224	1.025		1.0239
0.0085	0.9349	0.9368	0.9411	0.9491	1.0418	1.0283	1.0307		1.0289
0.0125	0.9417	0.9448	0.9476	0.9556	1.0494	1.0356	1.0378		1.0335
0.0175	0.9497	0.9508	0.9554	0.9624	1.0583	1.0444	1.0463		1.0474
0.0235	0.9562	0.9601	0.9645	0.9715	1.0688	1.0546	1.0563		1.0579
0.0305	0.9659	0.9708	0.9749	0.9799	1.0808	1.0664	1.0676		1.0699
0.0385	0.9767	0.9817	0.9865	0.9915	1.0965	1.0785	1.0823		1.0856
0.0475	0.9878	0.9938	0.9985	1.0045	1.1106	1.0924	1.1012		1.0997
0.0555	0.9979	1.0023	1.0069	1.0136	1.1224	1.1064	1.1165		1.1115
	303.15K				303.15K
0.0055	0.8461	0.8504	0.8547	0.8637	1.0312	1.0261	1.0293	1.0258
0.0085	0.8516	0.8558	0.8604	0.8674	1.0381	1.0325	1.0361	1.0306
0.0125	0.8586	0.8626	0.8674	0.8734	1.0466	1.0407	1.0446	1.0358
0.0175	0.8669	0.8707	0.8759	0.8829	1.0567	1.0505	1.0548	1.0493
0.0235	0.8747	0.8802	0.8858	0.8908	1.0687	1.0619	1.0668	1.0596
0.0305	0.8858	0.8911	0.8972	0.9021	1.0824	1.075	1.0804	1.0716
0.0385	0.8962	0.9021	0.9086	0.9132	1.1022	1.0914	1.0985	1.0874
0.0475	0.9072	0.9152	0.9202	0.9262	1.1217	1.1087	1.1185	1.1016
0.0555	0.9187	0.9267	0.9329	0.9399	1.1418	1.1293	1.1344	1.1137
	308.15K				308.15K
0.0055	0.769	0.7749	0.7817	0.7837	1.0344	1.0379	1.0391	1.035
0.0085	0.7752	0.7799	0.7869	0.7899	1.0434	1.0446	1.0461	1.0398
0.0125	0.7824	0.7862	0.7934	0.7954	1.0548	1.0531	1.0546	1.045
0.0175	0.7924	0.7957	0.8011	0.8057	1.0683	1.0631	1.0649	1.0585
0.0235	0.8015	0.8062	0.8102	0.8162	1.0843	1.0749	1.0769	1.0688
0.0305	0.8115	0.8177	0.8205	0.8255	1.1014	1.0884	1.0907	1.0808
0.0385	0.8202	0.8242	0.8312	0.8362	1.1132	1.1062	1.1048	1.0966
0.0475	0.8322	0.8382	0.8422	0.8482	1.1265	1.1156	1.1123	1.1108
0.0555	0.8457	0.8517	0.8547	0.8577	1.1398	1.1258	1.1221	1.1229
	313.15K				313.15K
0.0055	0.6832	0.6939	0.7056	0.7147	1.0293	1.0346	1.0398	1.037
0.0085	0.6901	0.7006	0.7125	0.7236	1.0396	1.0447	1.0498	1.0418
0.0125	0.701	0.7091	0.7211	0.7323	1.056	1.0573	1.0624	1.0473
0.0175	0.7127	0.7192	0.7323	0.7437	1.0735	1.0724	1.0776	1.0605
0.0235	0.7265	0.7356	0.7442	0.7562	1.0939	1.0901	1.0952	1.0708
0.0305	0.741	0.7496	0.7629	0.7735	1.1175	1.1102	1.1154	1.0828
0.0385	0.7613	0.7693	0.7814	0.7932	1.1256	1.1234	1.1278	1.0986
0.0475	0.7798	0.7928	0.8022	0.8139	1.1387	1.1343	1.1366	1.1128
0.0555	0.7974	0.8094	0.8178	0.8313	1.1475	1.1433	1.1458	1.1249

 

The B-coefficients were obtained from the linear plots using the least-square fitting method. The A- coefficient reflects solute-solute interaction (Pérez-Durán, 2019) and the B-coefficient reflect the solute-solvent interactions. Since in general, A/B <<1, the Jones –Dole equation reduces to,

η_r = l + β.C,                                         (4)

The relative viscosity data of these solutions have also been fitted in Moulik equation,

η_r ² = M + K C²                                     (5)

The density data of these solutions have also been fitted in Root’s equation,

(d – d₀) / C = R – SC^½                               (6)

where R and S are constants.

Table 4: Different parameters of KClO₃ in water and 1% KCl, KNO₃, NH₄NO₃ and KH₂PO₄ solution.

Temp	Massons Parameters		Jone-Dole’s Parameters		Moulik Parameters		Roots Parameter		‘β’ values	∆ (tr)
	cm3.mol-1	cm3.mol-1 L1/2	A/dm3/2mol-1/2	B/dm3.mol-1	K	M	R	S	β
KClO3 in Water
298.15K	121.3	-10.21	-0.01	0.32	12.61	1	0.24	0.29	0.28	0
303.15K	121.2	-8.85	-0.04	1.09	43.44	1.01	0.26	0.3	0.95	0
308.15K	121.9	-10.92	-0.05	2.01	84.38	1.03	0.24	0.27	1.81	0
313.15K	121.3	-10.19	-0.03	1.32	55.23	1.02	0.26	0.3	1.2	0
KClO3 in 1 % KCl
298.15K	121.7	-4.05	0.03	0.35	40.18	1.04	0.52	-1.39	0.87	0.4
303.15K	121.9	-4.03	0.05	0.93	55.7	1.03	0.53	-1.5	1.22	0.7
308.15K	122.1	-3.89	-0.03	1.58	74.91	1.03	0.54	-1.5	1.61	0.2
313.15K	122.2	-3.16	0.03	1.79	99.02	1.04	0.55	-1.6	2.1	0.9
KClO3 in 1 %   NH4NO3
298.15K	121.8	-7.71	0	1.14	52.04	1.02	1.45	-5.53	1.13	0.5
303.15K	122.1	-7.81	0.02	1.21	58.8	1.02	1.47	-5.7	1.27	0.9
308.15K	122.2	-7.56	0.01	1.52	72.89	1.03	1.28	-4.75	1.57	0.3
313.15K	122.4	-7.77	0.01	2.06	97.91	1.04	1.53	-6.03	2.08	1.1
KClO3 in 1%  KNO3
298.15K	121.9	-10.63	-0.03	1.57	57.27	1.03	1.45	-5.17	1.47	0.6
303.15K	122.1	-10.53	0.1	0.86	68.16	1.02	1.46	-5.21	1.24	0.9
308.15K	122.3	-10.69	0.06	1.17	64	1.03	1.5	-5.5	1.38	0.4
313.15K	122.6	-11.18	-0.02	1.94	86.68	1.03	1.39	-4.86	1.86	1.3
KClO3 in 1%  KH2PO4
298.15K	123.1	-10.25	0.02	1.57	56.32	1.03	1.46	-5.27	1.27	1.8
303.15K	123.3	-9.73	0.15	0.86	66.17	1.02	1.45	-5.23	1.23	2.1
308.15K	123.5	-10.55	0.03	1.17	71.24	1.03	1.53	-5.51	1.27	1.6
313.15K	123.7	-10.7	0.02	1.94	89.35	1.03	1.29	-4.76	1.46	2.4

The diffusion controlled reaction rate constant k_d can be evaluated by using the viscosity data as (Rathi & Nikumbh, 2019)

The evaluated values are used to predict whether the solvolysis is fast or slow process.

Table 5: Diffusion reaction rate constant k_d (L mol^-1 s^-1) values of KClO₃ water and 1 % KCl, KNO₃, NH₄NO₃ and KH₂PO₄ solution.

Molar Conc. mol/dm3	KClO3 in Water	KClO3 in   1% KCl	KClO3 in 1% NH4NO3	KClO3 in   1% KNO3	KClO3   1% KH2PO4	KClO3 in Water	KClO3  in 1% KCl	KClO3 in 1% NH4NO3	KClO3 in   1% KNO3	KClO3    1% KH2PO4
298.15K						298.15K
0.0055	7.38	7.23	7.21	7.18	7.16	9.35	9.12	9.05	8.97	8.21
0.0085	7.37	7.21	7.18	7.14	7.13	9.28	9.06	9.01	8.92	8.14
0.0125	7.36	7.18	7.14	7.09	7.06	9.2	8.99	8.93	8.86	7.92
0.0175	7.35	7.14	7.09	7.03	7.04	9.1	8.91	8.85	8.79	7.84
0.0235	7.34	7.11	7.03	6.96	6.94	8.99	8.81	8.75	8.71	7.74
0.0305	7.32	7.09	6.97	6.88	6.86	8.87	8.7	8.65	8.62	7.65
0.0385	7.31	7.06	6.83	6.74	6.73	7.91	7.83	8.56	8.38	7.56
0.0475	7.3	7.04	6.76	6.56	6.56	7.87	7.71	8.34	8.17	7.38
0.0555	7.29	7.01	6.45	6.43	6.4	7.68	7.64	8.11	8.01	7.29
303.15K						303.15K
0.0055	8.27	8.09	8.03	7.98	8.19	10.55	10.28	10.12	10.12	10.23
0.0085	8.24	8.05	7.99	7.94	8.04	10.5	10.19	10.05	10.05	10.14
0.0125	8.2	8.01	7.94	7.9	7.89	10.44	10.09	9.96	9.96	9.95
0.0175	8.15	7.95	7.88	7.84	7.74	10.37	9.97	9.85	9.85	9.86
0.0235	8.1	7.88	7.82	7.77	7.63	10.28	9.83	9.73	9.73	9.72
0.0305	8.04	7.81	7.74	7.7	7.55	10.19	9.68	9.59	9.59	9.68
0.0385	7.89	7.23	7.66	7.68	7.46	10	9.46	9.33	9.47	9.57
0.0475	7.67	7.11	7.54	7.43	7.31	9.89	9.32	9.24	9.33	9.45
0.0555	7.43	6.89	7.23	7.1	7.2	9.76	9.21	9.12	9.28	9.29

 

Result and Discussion

The values of densities and viscosities of KClO₃ solutions decrease with increase in temperature and increases with increase in concentration. The apparent molar volume values of ∅_V decrease with concentration while the relative viscosities are found to increase with concentrations. The ∅_V⁰ values of KClO₃ under investigation in all solvent systems are large and positive. The Sv is negative .These results indicate that there is presence of strong solute-solute interactions. (Shekaari, 2019) The Diffusion reaction rate constant (kd) values are positive and decrease with increase in temperature as well as concentration. Positive Kd values reveals that the solvolysis of KClO₃ in aqueous electrolyte studied is diffusion controlled rather than activated controlled process.

Conclusion

The increase in densities and viscosities with concentration may be due to strengthening of solute-solvent interactions. (Gupta, 2019). All the investigated parameters has been revealed that there exist strong solute– solvent interaction. This molecular interaction data help to reveal the toxicity of chlorate. When chlorate is added in the soil or injected in the stem of Longan plants ,it creates a strong solute –solvent interaction with the other aqueous ionic solids which are already present in the soil or plant tissues. Chlorate acts as a structure maker and form a tight solvation layer as well as high compactness around the solute. Over-application of flower-inducing chlorate failed to induce flower but caused toxic effects such as leaf chlorosis and drop in longan. The solvolysis of KClO₃ in water and KNO₃ or other nitrate and phosphate solutions at different temperatures is diffusion controlled process. The co-sphere of solvent significantly suppressed nitrate reducing activity in the leaves. This suggested that chlorate not only inhibited photosynthesis due to stomata closure but also due to breakdown of photosynthetic apparatus in chloroplasts. (Sritontip C. Y., 1999) The higher values of densities of KClO₃ in KCl, KNO₃ ,NH₄NO₃   and KH₂PO₄ are due to the relative salvation, corresponding relative volumes of system and molar mass of the salts. Strong molecular interactions induces chlorate stress (LU Jiemei, 2017) due to occurrence of osmotic adjustment which results in massive accumulation of soluble amino acids and sugars. Excessive use of chlorate as a bleaching agent toxifies the water (Lubbers, Chauhan , & Bianchine , 1981), soil and disturbs the environment’s equilibrium. (Kanitz , 1996). Reducing the usage of chlorate, used in the production of colours, safety matches, and explosives for tanning and finishing leather, is important in order to conserve and save the environment.

Acknowledgement

I would like to sincerely acknowledge the guidance and help provided by Dr. Arun B. Nikumbh for compilation of this research report.

Conflict of Interest

There is no conflict of interest.

Funding sources

There is no funding source.

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