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Discoveries in Agriculture and Food Sciences - Vol. 12, No. 4

Publication Date: August 25, 2024

DOI:10.14738/dafs.124.16859.

Kaewsrichan, J., Wongwitwichot, P., Tipmanee, V., & Pengnoo, A. (2024). Productive Growing System of Andrographis Paniculata

and Inhibitions of Reverse Transcriptase and 3clpro Enzymes by the Isolated Andrographolide. Discoveries in Agriculture and Food

Sciences, 12(4). 21-34.

Services for Science and Education – United Kingdom

Productive Growing System of Andrographis Paniculata and

Inhibitions of Reverse Transcriptase and 3clpro Enzymes by the

Isolated Andrographolide

Jasadee Kaewsrichan

Department of Pharmaceutical Chemistry and Drug Delivery System Excellence

Center, Faculty of Pharmaceutical Sciences, Prince of Songkla University, Hat-Yai,

Songkhla, 90112, Thailand

Paweena Wongwitwichot

Department of Pharmaceutical Chemistry and Drug Delivery System Excellence

Center, Faculty of Pharmaceutical Sciences, Prince of Songkla University, Hat-Yai,

Songkhla, 90112, Thailand

Varomyalin Tipmanee

Department of Biomedical Sciences and Bioengineering, Faculty of Medicine,

Prince of Songkla University, Hat-Yai, Songkhla, 90112, Thailand

Ashara Pengnoo

Department of Earth Science, Faculty of Natural Resources,

Prince of Songkla University, Hat Yai, Songkhla 90112, Thailand

ABSTRACT

Molecular interactions between andrographolide (ADP) and proteins/enzymes of

different pathogenic viruses were computationally predicted by using docking

method. Binding energy corresponded to a protein-ADP pairing was theoretically

accounted in comparison with other current antiviral drugs as positive ligands. In

silico, interactions between ADP and PLpro (PDB, 6WX4), ADP and 3CLpro (PDB,

7LMD), ADP and ACE-2 receptor-spike protein complex (PDB, 6M0J), as well as ADP

and M2 protein (PDB, 6BKK) were stronger than those of between rimantadine,

remdesivir, lopinavir, or ritonavir and the described proteins. The inhibitions of

ADP against reverse transcriptase and 3CLpro activities were greater than those of

lopinavir, ritonavir, and oseltamivir, according to in vitro assays. ADP was isolated

as a major active compound from Andrographis paniculata grown outdoor in newly

established, cost-effective, hydroponic system. An average fresh mass per plant was

as high as 170 g from a 35x35 cm2 spacing hole. Simple and productive procedures

were recently suggested for ADP extraction. These acquired data would be applied

for pharmaceutical manufacturing.

Keywords Andrographis paniculate, Andrographolide, Molecular docking, Reverse

transcription, 3C rhinoviral protease, Outdoor hydroponic system

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Discoveries in Agriculture and Food Sciences (DAFS) Vol 12, Issue 4, August- 2024

Services for Science and Education – United Kingdom

INTRODUCTION

Viruses are biological entities capable of replication in living organisms only. Distinct

mechanisms have been used by a virus to affect an organism. This is why a virus that causes

illness in cats may not infect humans. There are serious and persistent threats from viruses to

humankind at present, due to the emergence, re-emergence, or evolution of drug-resistant

strains. Consequently, continuous search of new and potent antiviral drugs is important. Viral

life cycle is termed for a group of stages used by a virus to infect cells. These include (i),

attachment to host cell membrane; (ii), entry into host cells; (iii), genome uncoating, replication,

transcription, and translation; (iv), assembly; and (v), budding and release. Each stage is

completed by particular enzymes, which indicated to be dependent on the genome of the

infected virus. For instance, replication of most DNA viruses arises in the host cell nucleus and

is carried out by the host enzymes. Another large DNA virus, called Vaccinia, is an exception in

that replication and transcription occur in the host cell cytoplasm using enzymes encoded by

the infected virus. Genetic information of RNA viruses is stored in the form of RNA molecules.

Their replication can be achieved by means of RNA-dependent RNA polymerase (RdRp) or

RNA-dependent DNA polymerase (so-called reverse transcriptase) for RNA or cDNA synthesis,

respectively. Indeed, the viruses must encode reverse transcriptase on their own because of not

available from cells of humans. Then, integration between the cDNA and the host genome can

be happened, leaving the viral genome persistent in the infected host cells. Consequently, it is

helpful to hinder viral infection, replication, and spreading by inactivation of these associating

enzymes [1], which have been drug targets for searching new lead compounds by

computational methodology.

Andrographolide (ADP) is a major secondary metabolite of Andrographis paniculata with

diterpenoids structure. The herb has been used in traditional Eastern medicine for treatments

such as common cold, sore throat, liver disease, jaundice, diabetes, dysentery, chronic malaria,

and snake bite [2,3], and be included in Thai Herbal Pharmacopoeia since 2017. Few years ago,

the potentials of ADP and the A. paniculata extracts against SARS-CoV-2 were reported [4]. Hard

capsules containing dried powder or extracts of the herb were dispensed to COVID-19 patients

with mild symptoms in Thailand of which the treatment outcomes were desirable. Later,

different interactions between ADP and structural or non-structural proteins of SARS-CoV-2

such as papain-like protease, coronavirus main proteinase, and the spike protein, were

demonstrated by many in silico researches [5]. By network pharmacological analysis, immune

modulatory effects of ADP on p53 signaling and chemokines/natural killer cell mediating

cytotoxicity have been apparent, including its inhibitions towards infectious viral strains like

herpes simplex virus 1, human immunodeficiency virus, influenza A virus, hepatitis C virus, as

well as dengue virus. So far, broad inhibitory spectra of ADP have been indicated [6]. However,

molecular mechanisms that underline the described therapeutic actions of ADP are scant at

present, leading to the discoveries important.

In this research, molecular docking method was carried out to predict what proteins/enzymes

of human infectious strains of viruses are potential as ADP targets. By comparing with other

commonly used antiviral drugs, possible/attractive interactions based on binding energy

(kcal/mole) could be suggested. Two enzymatic assays [7] were performed in vitro for insisting

the computationally simulated results. The recently used ADP was purified from A. paniculata

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Kaewsrichan, J., Wongwitwichot, P., Tipmanee, V., & Pengnoo, A. (2024). Productive Growing System of Andrographis Paniculata and Inhibitions of

Reverse Transcriptase and 3clpro Enzymes by the Isolated Andrographolide. Discoveries in Agriculture and Food Sciences, 12(4). 21-34.

URL: http://dx.doi.org/10.14738/dafs.124.16859

grown outdoor in our modified hydroponic garden. Purity and content of the ADP were

demonstrated by using HPLC technique [8]. Using our developed procedures for plating A.

paniculata and extracting ADP, it seemed to increase yield and quality of the extracted ADP

(closures on planting of A. paniculata and purification of ADP by two petty patents). The

obtained data might be applicable in producing a pharmaceutical grade of ADP for

manufacturing scale.

METHODS

Chemicals and Reagents

Chemicals and solvents of analytical/chromatographic grades were used. Methanol and

absolute ethanol were bought from Merck (Darmstadt, Germany). ADP working standard

(98.15% purity) was obtained from Department of Medical Sciences Reference Standards,

Ministry of Public Health, Thailand. Abacavir sulfate, lopinavir, ritonavir, and oseltamivir

phosphate were purchased from Sigma-Aldrich. Mouse muscle cell line, C2C12, was acquired

from ATCC. Chemicals/reagents for cell culture technique such as Dulbecco’s Modified Eagle

medium (DMEM), fetal bovine serum (FBS), penicillin/streptomycin, fungizone, RIPA buffer,

etc., were purchased from Gibco (Life Technologies, NY, USA). Oligonucleotide primers were

ordered from Macrogen HQ (Seoul, Republic of Korea). The HRV 3C protease activity assay kit

(Colorimetric) was bought from BioVision (MA, USA).

Molecular Docking Study

Three-dimensional structures of ADP (Pubchem ID: 5318517) and oseltamivir (Pubchem ID:

65028) were downloaded from PubChem database, while those of lopinavir (ChemSpider ID:

83706) and ritonavir (ChemSpider ID: 347980) were from ChemSpider server. Translation to

Protein Data Bank (PDB) format files by using Online SMILES Translator and Structure File

Generator (https://cactus.nci.nih.gov/translate/) was then performed. Crystal structures of

enzymes were acquired from RCSB protein database (http://www.rcsb.org). These included

influenza A neuraminidases: H1N1 (PDB ID: 6HP0), H3N2 (PDB ID: 4GZT), H3N8 (PDB ID:

4WA4), N4 (PDB ID: 2HTW); influenza A M2 protein (PDB ID: 6BKK); hepatitis C virus

nonstructural protein 5B (NS5B) isolate 1 (PDB ID: 4TLR) and subtype 1b (PDB ID: 5CZB);

hepatitis B virus mutant capsid proteins: (PDB ID: 5T2P) and (PDB ID: 6J10); SARS CoV-2

proteases: 3-chymotrypsin-like protease (PDB ID:7LMD) and papain-like protease (PDB ID:

6WX4); and ACE-2 receptor-spike protein complex (PDB ID: 6M0J). Any attached molecules

including water were dissected from the crystal structures. But polar hydrogen atoms were

added. These were operated by using AutoDock4. Files of target proteins and test ligands were

saved as PDBQT format for molecular docking. Again, AutoDock4 was used for selection of

active site residues and molecular docking Grid, and docking protocols of the active site

predictions. Grid site was set spacing at 0.375 Å. The x-y-z dimensions were set at 120-120-120

Å3. The rigid entity of protein structures was used. But the ligand was set as a flexible molecule.

Docking study was rendered by using the Lamarckian genetic algorithm (GA) and implemented

by AutoDock4. The number of GA runs was 50 with a popular size of 200. Binding energy

(ΔGbind) was analyzed by using ADT. Interactions were visualized by using BIOVIA Discovery

Studio (BIOVIA, 2020). Protein-ligand structure at the binding site was visualized by using

Visual Molecular Dynamics (VMD) package.