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Frontiers of Chemical Science and Engineering

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, Volume 11 Issue 4 Previous Issue   
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COMMUNICATION
Enzyme-instructed self-assembly of peptides containing phosphoserine to form supramolecular hydrogels as potential soft biomaterials
Jie Zhou, Xuewen Du, Jiaqing Wang, Natsuko Yamagata, Bing Xu
Front. Chem. Sci. Eng.. 2017, 11 (4): 509-515.   DOI: 10.1007/s11705-017-1613-7
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Enzyme-instructed self-assembly (EISA) offers a facile approach to explore the supramolecular assemblies of small molecules in cellular milieu for a variety of biomedical applications. One of the commonly used enzymes is phosphatase, but the study of the substrates of phosphatases mainly focuses on the phosphotyrosine containing peptides. In this work, we examine the EISA of phosphoserine containing small peptides for the first time by designing and synthesizing a series of precursors containing only phosphoserine or both phosphoserine and phosphotyrosine. Conjugating a phosphoserine to the C-terminal of a well-established self-assembling peptide backbone, (naphthalene-2-ly)-acetyl-diphenylalanine (NapFF), affords a novel hydrogelation precursor for EISA. The incorporation of phosphotyrosine, another substrate of phosphatase, into the resulting precursor, provides one more enzymatic trigger on a single molecule, and meanwhile increases the precursors’ propensity to aggregate after being fully dephosphorylated. Exchanging the positions of phosphorylated serine and tyrosine in the peptide backbone provides insights on how the specific molecular structures influence self-assembling behaviors of small peptides and the subsequent cellular responses. Moreover, the utilization of D-amino acids largely enhances the biostability of the peptides, thus providing a unique soft material for potential biomedical applications.

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VIEWS & COMMENTS
Oral product input to the GI tract: GIS an oral product performance technology
Gordon L. Amidon, Yasuhiro Tsume
Front. Chem. Sci. Eng.. 2017, 11 (4): 516-520.   DOI: 10.1007/s11705-017-1658-7
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The patient receives a pharmaceutical product, not a drug. The pharmaceutical products are formulated with a drug, an active ingredient to produce the maximum therapeutic effect after oral absorption. Therefore, it is the product we must optimize for the patients. In order to assure the safety and efficacy of pharmaceutical products, we need an in vivo predictive tool for oral product performance in patients. Currently, we are a surprisingly long way from accomplishing that objective. If the 20th century was the ‘age of the drug’, i.e., the ‘magic bullet’, the 21st century must become the ‘age of the guided missile’, i.e., the delivery system, including the form of the active pharmaceutical ingredient (API) (‘drug’). The physical form of the drug and the delivery system must be optimized to maximize the therapeutic benefits of pharmaceutical products for humans. Oral immediate release (IR) dosage forms cannot be optimal for all drugs or likely even any drugs (APIs). Still, the formulation of pharmaceutical products has to be optimized for patients. But how do we optimize oral delivery of drugs? It is usually through ‘trial and error’, in humans! We need a better way to optimize the oral dosage forms. We have suggested to select different dissolution methodologies for this optimization based on BCS Subclasses. In this article, we present the predicted in vivo drug dissolution profile of ketoconazole as a model drug from our laboratory utilizing a gastrointestinal simulator (GIS), which is an adaptation of the ASD system. GIS consists of three chambers representing stomach, duodenum, and jejunum, to create the human gastrointestinal tract-like environment and enable the control the gastric emptying rate. This dissolution system allows the monitoring of the drug dissolution phenomena and the observation of the supersaturation and the precipitation of pharmaceutical products, which is useful information to predict in vivo dissolution of pharmaceutical products. This system can provide the actual input needed to accurately predict the input into the systemic circulation required by many of the absorption prediction packages available today.

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RESEARCH ARTICLE
Gene delivery into isolated Arabidopsis thaliana protoplasts and intact leaves using cationic, α-helical polypeptide
Nan Zheng, Ziyuan Song, Yang Liu, Lichen Yin, Jianjun Cheng
Front. Chem. Sci. Eng.. 2017, 11 (4): 521-528.   DOI: 10.1007/s11705-017-1612-8
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The application of gene delivery materials has been mainly focused on mammalian cells while rarely extended to plant engineering. Cationic polymers and lipids have been widely utilized to efficiently deliver DNA and siRNA into mammalian cells. However, their application in plant cells is limited due to the different membrane structures and the presence of plant cell walls. In this study, we developed the cationic, α-helical polypeptide that can effectively deliver DNA into both isolated Arabidopsis thaliana protoplasts and intact leaves. The PPABLG was able to condense DNA to form nanocomplexes, and they exhibited significantly improved transfection efficiencies compared with commercial transfection reagent Lipofectamine 2000 and classical cell penetrating peptides such as poly(L-lysine), HIV-TAT, arginine9, and poly(L-arginine). This study therefore widens the utilities of helical polypeptide as a unique category of gene delivery materials, and may find their promising applications toward plant gene delivery.

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Aptamer-coded DNA nanoparticles for targeted doxorubicin delivery using pH-sensitive spacer
Pengwei Zhang, Junxiao Ye, Ergang Liu, Lu Sun, Jiacheng Zhang, Seung Jin Lee, Junbo Gong, Huining He, Victor C. Yang
Front. Chem. Sci. Eng.. 2017, 11 (4): 529-536.   DOI: 10.1007/s11705-017-1645-z
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An anticancer drug delivery system consisting of DNA nanoparticles synthesized by rolling circle amplification (RCA) was developed for prostate cancer membrane antigen (PSMA) targeted cancer therapy. The template of RCA was a DNA oligodeoxynucleotide coded with PSMA-targeted aptamer, drug-loading domain, primer binding site and pH-sensitive spacer. Anticancer drug doxorubicin, as the model drug, was loaded into the drug-loading domain (multiple GC-pair sequences) of the DNA nanoparticles by intercalation. Due to the integrated pH-sensitive spacers in the nanoparticles, in an acidic environment, the cumulative release of doxorubicin was far more than the cumulative release of the drug in the normal physiological environment. In cell uptake experiments, treated with doxorubicin loaded DNA nanoparticles, PSMA-positive C4-2 cells could take up more doxorubicin than PSMA-null PC-3 cells. The prepared DNA nanoparticles showed the potential as drug delivery system for PSMA targeting prostate cancer therapy.

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Sorption enhanced catalytic CF4 hydrolysis with a three-stage catalyst-adsorbent reactor
Jae-Yun Han, Chang-Hyun Kim, Boreum Lee, Sung-Chan Nam, Ho-Young Jung, Hankwon Lim, Kwan-Young Lee, Shin-Kun Ryi
Front. Chem. Sci. Eng.. 2017, 11 (4): 537-544.   DOI: 10.1007/s11705-017-1651-1
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In this study, we developed a three-stage catalyst-adsorbent reactor for the catalytic hydrolysis of CF4. Each stage is composed of a catalyst bed followed by an adsorbent bed using Ca(OH)2 to remove HF. The three stages are connected in series to enhance the hydrolysis of CF4 and eliminate a scrubber to dissolve HF in water at the same time. With a 10 wt-% Ce/Al2O3 catalyst prepared by the incipient wetness method using boehmite and a granular calcium hydroxide as an adsorbent, the CF4 conversion in our proposed reactor was 7%–23% higher than that in a conventional single-bed catalytic reactor in the temperature range of 923–1023 K. In addition, experimental and numerical simulation (Aspen HYSYS®) results showed a reasonable trend of increased CF4 conversion with the adsorbent added and these results can be used as a useful design guideline for our newly proposed multistage reactor system.

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Effects of metal ions on the morphology of calcium sulfate hemihydrate whiskers by hydrothermal method
Tianjie Liu, Hao Fan, Yanxia Xu, Xingfu Song, Jianguo Yu
Front. Chem. Sci. Eng.. 2017, 11 (4): 545-553.   DOI: 10.1007/s11705-017-1665-8
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The effects of Na+, Mg2+, Al3+ and Fe3+ ion concentrations on the crystal morphology of calcium sulfate hemihydrate whiskers formed via a hydrothermal method have been studied. In the presence of Al3+ concentrations higher than 1×103 mol/L the whiskers were significantly shorter and thicker and the presence of Mg2+ and Fe3+ resulted in shorter whiskers. The presence of Na+ did not affect the morphology of the whiskers. Through elemental analysis, it was determined that Mg2+ and Al3+ were selectively adsorbed on the surfaces of the crystals, whereas Fe3+ underwent a hydrolysis reaction to form a brown precipitate which decreased the ion concentration in the solution. These results indicate that in raw materials used for the industrial preparation of calcium sulfate whiskers, Al3+ and Fe3+ should be removed and the Mg2+ concentration should be less than 8 × 103 mol/L in order to obtain pure whiskers with high aspect ratios.

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Preparation and characteristics of TEMPO-oxidized cellulose nanofibrils from bamboo pulp and their oxygen-barrier application in PLA films
Bozhen Wu, Biyao Geng, Yufei Chen, Hongzhi Liu, Guangyao Li, Qiang Wu
Front. Chem. Sci. Eng.. 2017, 11 (4): 554-563.   DOI: 10.1007/s11705-017-1673-8
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Bleached bamboo kraft pulp was pretreated by 2,2,6,6-tetramethylpiperidine-1-oxy radical (TEMPO)-mediated oxidation using a TEMPO/NaBr/NaClO system at pH= 10 in water to facilitate mechanical disintegration into TEMPO-oxidized cellulose nanofibrils (TO-CNs). A series of TO-CNs with different carboxylate contents were obtained by varying amounts of added NaClO. An increase in carboxylate contents results in aqueous TO-CN dispersions with higher yield, zeta potential values, and optical transparency. When carboxylate groups are introduced, the DPv value of the TO-CNs remarkably decreases and then levels off. And the presence of hemicellulose in the pulp is favorable to TEMPO oxidization. After the oxidization, the native cellulose I crystalline structure and crystal size of bamboo pulp are almost maintained. TEM micrographs revealed that the degree of nanofibrillation is directly proportional to the carboxylate contents. With increasing carboxylate contents, the free-standing TO-CN films becomes more transparent and mechanically stronger. The oxygen permeability of PLA films drastically decreases from 355 for neat PLA to 8.4 mL·m−2·d1 after coating a thin layer of TO-CN with a carboxylate content of 1.8 mmol·g−1. Therefore, inexpensive and abundant bamboo pulp would be a promising starting material to isolate cellulose nanfibrils for oxygen-barrier applications.

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The effect of doping and steam treatment on the catalytic activities of nano-scale H-ZSM-5 in the methanol to gasoline reaction
Baodong Song, Yongqiang Li, Gang Cao, Zhenhai Sun, Xu Han
Front. Chem. Sci. Eng.. 2017, 11 (4): 564-574.   DOI: 10.1007/s11705-017-1654-y
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In the transformation of methanol to gasoline (MTG), the selectivity to gasoline and the aromatic content in the produced gasoline are important factors. The catalytic activities of steam-treated and non-steam-treated nano-scale H-ZSM-5 (NHZ5) catalysts impregnated with Ag(I), Zn(II) or P(V) have been investigated in a continuous flow fixed bed reactor. The NH3-TPD results showed that after impregnation, the Ag/NHZ5, Zn/NHZ5 and P/NHZ5 catalysts contained comparatively more strong, medium-strong and weak acid sites, respectively. Treatment with steam decreased the number of acid sites in all the catalysts, but the pore volumes in the catalysts were larger which improved carbon deposition resistance resulting in prolonged lifetimes. After 6 h of MTG reaction, the selectivity to gasoline for the steam-treated catalysts, AgH2O/NHZ5, ZnH2O/NHZ5 and PH2O/NHZ5 were 70.5, 68.4 and 68.7 wt-%, respectively, whereas their respective aromatic contents in the produced gasoline were 61.9, 55.4 and 39.0 wt-%. Thus PH2O/NHZ5 is the most promising catalyst for MTG applications which can meet the China IV gasoline standard that the amount of aromatics in gasoline should be less than 48 wt-%.

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Chitosan/polyethylene glycol impregnated activated carbons: Synthesis, characterization and adsorption performance
Ehsan Salehi, Fereshteh Soroush, Maryam Momeni, Aboulfazl Barati, Ali Khakpour
Front. Chem. Sci. Eng.. 2017, 11 (4): 575-585.   DOI: 10.1007/s11705-017-1650-2
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Novel modified activated carbons (ACs) with enhanced adsorptive properties were obtained coating by chitosan (CS), polyethylene glycol (PEG) and blends of the two polymers (0:1, 1:0, 1:1, 1:2 and 2:1 wt/wt) on ACs by an impregnation technique. The adsorption performances of the pristine, acidified and polymer-impregnated ACs were studied using methylene blue as a model adsorbate. The adsorbents were characterized using Fourier transform infrared spectroscopy, scanning electron microscopy and abrasion hardness tests. The average coating thicknesses were between 10 to 23 microns. The pore sizes, pore densities and pore capacities of the activated carbons increased as the wt-% PEG in the coating increased. The highest adsorption capacity (424.7 mg/g) was obtained for the chitosan-coated ACs and this adsorption was well described by the Langmuir isotherm model. The kinetic results were best described by the pseudo-second-order kinetic model. The highest rate constant was obtained with the ACs modified with the CS:PEG (2:1) coating and this result was almost 2.6 times greater than that of the unmodified ACs. The CS/PEG impregnated ACs also displayed superior hardness (~90%), compared to unmodified ACs (~85%). Overall the chitosan had a greater effect on improving adsorption capacity whereas the polyethylene glycol enhanced the adsorption rate.

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Rh2O3/hexagonal CePO4 nanocatalysts for N2O decomposition
Huan Liu, Zhen Ma
Front. Chem. Sci. Eng.. 2017, 11 (4): 586-593.   DOI: 10.1007/s11705-017-1659-6
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Hexagonal CePO4 nanorods were prepared by a precipitation method and hexagonal CePO4 nanowires were prepared by hydrothermal synthesis at 150 °C. Rh(NO3)3 was then used as a precursor for the impregnation of Rh2O3 onto these CePO4 materials. The Rh2O3 supported on the CePO4 nanowires was much more active for the catalytic decomposition of N2O than the Rh2O3 supported on CePO4 nanorods. The stability of both catalysts as a function of time on stream was studied and the influence of the co-feed (CO2, O2, H2O or O2/H2O) on the N2O decomposition was also investigated. The samples were characterized by N2 adsorption-desorption, inductively coupled plasma optical emission spectroscopy, X-ray diffraction, transmission electron microscopy, X-ray photoelectron microscopy, hydrogen temperature-programmed reduction, oxygen temperature-programmed desorption, and CO2 temperature-programmed desorption in order to correlate the physicochemical and catalytic properties.

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Metal-organic framework loaded manganese oxides as efficient catalysts for low-temperature selective catalytic reduction of NO with NH3
Minhua Zhang, Baojuan Huang, Haoxi Jiang, Yifei Chen
Front. Chem. Sci. Eng.. 2017, 11 (4): 594-602.   DOI: 10.1007/s11705-017-1668-5
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A mild in-situdeposition method was used to fabricate Mn-based catalysts on a UiO-66 carrier for the selective catalytic reduction of NO by NH3 (NH3-SCR). The catalyst with 8.5 wt-% MnOx loading had the highest catalytic activity for NH3-SCR with a wide temperature window (100–290 °C) for 90% NO conversion. Characterization of the prepared MnOx/UiO-66 catalysts showed that the catalysts had the crystal structure and porosity of the UiO-66 carrier and that the manganese particles were well-distributed on the surface of the catalyst. X-ray photoelectron spectroscopy analysis showed that there are strong interactions between the MnOx and the Zr oxide secondary building units of the UiO-66 which has a positive effect on the catalytic activity. The 8.5 wt-% MnOx catalyst maintained excellent activity during a 24-h stability test and exhibited good resistance to SO2 poisoning.

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Effects of preparation methods on the activity of CuO/CeO2 catalysts for CO oxidation
Huanhuan Shang, Xiaoman Zhang, Jing Xu, Yifan Han
Front. Chem. Sci. Eng.. 2017, 11 (4): 603-612.   DOI: 10.1007/s11705-017-1661-z
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CO oxidation has been investigated on three CuO/CeO2 catalysts prepared by impregnation, co-precipitation and mechanical mixing. The origin of active sites was explored by the multiple techniques. The catalyst prepared by impregnation has more highly dispersed CuO and stronger interactions between CuO and CeO2 to promote the reduction of CuO to Cu+ species at the Cu-Ce interface, leading to its highest catalytic activity. For the catalyst prepared by co-precipitation, solid solution structures observed in Raman spectra suppress the formation of the Cu-Ce interface, where the adsorbed CO will react with active lattice oxygen to form CO2, and thus it displays a lower catalytic performance. No Cu-Ce interface exists in the catalyst prepared by the mechanical mixing method due to the separate phases of CuO and CeO2, resulting in its lowest activity among the three catalysts.

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Bimetallic Ni-Fe catalysts derived from layered double hydroxides for CO methanation from syngas
Honggui Tang, Shuangshuang Li, Dandan Gong, Yi Guan, Yuan Liu
Front. Chem. Sci. Eng.. 2017, 11 (4): 613-623.   DOI: 10.1007/s11705-017-1664-9
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Carbon deposition and sintering of active components such as nano particles are great challenges for Ni-based catalysts for CO methanation to generate synthetic natural gas from syngas. Facing the challenges, bimetallic catalysts with different Fe content derived from layered double hydroxide containing Ni, Fe, Mg, Al elements were prepared by co-precipitation method. Nanoparticles of Ni-Fe alloy were supported on mixed oxides of aluminium and magnesium after calcination and reduction. The catalysts were characterized by Brunner-Emmett-Teller (BET), X-ray diffraction, hydrogen temperature programmed reduction, inductively coupled plasma, X-ray photoelectron spectroscopy, transmission electron microscopy and thermogravimetric techniques, and their catalytic activity for CO methanation was investigated. The results show that the Ni-Fe alloy catalysts exhibit better catalytic performance than monometallic catalysts except for the Ni4Fe-red catalyst. The Ni2Fe-red catalyst shows the highest CO conversion (100% at 260–350 °C), as well as the highest CH4 selectivity (over 95% at 280–350 °C), owing to the formation of Ni-Fe alloy. In stability test, the Ni2Fe-red catalyst exhibits great improvement in both anti-sintering and resistance to carbon formation compared with the Ni0Fe-red catalyst. The strong interaction between Ni and Fe element in alloy and surface distribution of Fe element not only inhibits the sintering of nanoparticles but restrains the formation of Ni clusters.

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REVIEW ARTICLE
Engineering platelet-mimicking drug delivery vehicles
Quanyin Hu, Hunter N. Bomba, Zhen Gu
Front. Chem. Sci. Eng.. 2017, 11 (4): 624-632.   DOI: 10.1007/s11705-017-1614-6
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Platelets dynamically participate in various physiological processes, including wound repair, bacterial clearance, immune response, and tumor metastasis. Recreating the specific biological features of platelets by mimicking the structure of the platelet or translocating the platelet membrane to synthetic particles holds great promise in disease treatment. This review highlights recent advancements made in the platelet-mimicking strategies. The future opportunities and translational challenges are also discussed.

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Functional ferritin nanoparticles for biomedical applications
Zhantong Wang, Haiyan Gao, Yang Zhang, Gang Liu, Gang Niu, Xiaoyuan Chen
Front. Chem. Sci. Eng.. 2017, 11 (4): 633-646.   DOI: 10.1007/s11705-017-1620-8
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Ferritin, a major iron storage protein with a hollow interior cavity, has been reported recently to play many important roles in biomedical and bioengineering applications. Owing to the unique architecture and surface properties, ferritin nanoparticles offer favorable characteristics and can be either genetically or chemically modified to impart functionalities to their surfaces, and therapeutics or probes can be encapsulated in their interiors by controlled and reversible assembly/disassembly. There has been an outburst of interest regarding the employment of functional ferritin nanoparticles in nanomedicine. This review will highlight the recent advances in ferritin nanoparticles for drug delivery, bioassay, and molecular imaging with a particular focus on their biomedical applications.

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Progress in membrane distillation crystallization: Process models, crystallization control and innovative applications
Xiaobin Jiang, Linghan Tuo, Dapeng Lu, Baohong Hou, Wei Chen, Gaohong He
Front. Chem. Sci. Eng.. 2017, 11 (4): 647-662.   DOI: 10.1007/s11705-017-1649-8
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Membrane distillation crystallization (MDC) is a promising hybrid separation process that has been applied to seawater desalination, brine treatment and wastewater recovery. In recent years, great progress has been made in MDC technologies including the promotion of nucleation and better control of crystallization and crystal size distribution. These advances are useful for the accurate control of the degree of supersaturation and for the control of the nucleation kinetic processes. This review focuses on the development of MDC process models and on crystallization control strategies. In addition, the most important innovative applications of MDC in the last five years in crystal engineering and pharmaceutical manufacturing are summarized.

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Molecular engineering of dendrimer nanovectors for siRNA delivery and gene silencing
Yu Cao, Xiaoxuan Liu, Ling Peng
Front. Chem. Sci. Eng.. 2017, 11 (4): 663-675.   DOI: 10.1007/s11705-017-1623-5
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Small interfering RNA (siRNA) therapeutics hold great promise to treat a variety of diseases, as long as they can be delivered safely and effectively into cells. Dendrimers are appealing vectors for siRNA delivery by virtue of their well-defined molecular architecture and multivalent cooperativity. However, the clinical translation of RNA therapeutics mediated by dendrimer delivery is hampered by the lack of dendrimers that are of high quality to meet good manufacturing practice standard. In this context, we have developed small amphiphilic dendrimers that self-assemble into supramolecular structures, which mimic high-generation dendrimers synthesized with covalent construction, yet are easy to produce in large amount and superior quality. Indeed, the concept of supramolecular dendrimers has proved to be very promising, and has opened up a new avenue for dendrimer-mediated siRNA delivery. A series of self-assembling supramolecular dendrimers have consequently been established, some of them out-performing the currently available nonviral vectors in delivering siRNA to various cell types in vitro and in vivo, including human primary cells and stem cells. This short review presents a brief introduction to RNAi therapeutics, the obstacles to their delivery and the advantages of dendrimer delivery vectors as well as our bio-inspired structurally flexible dendrimers for siRNA delivery. We then highlight our efforts in creating self-assembling amphiphilic dendrimers to construct supramolecular dendrimer nanosystems for effective siRNA delivery as well as the related structural alterations to enhance delivery efficiency. The advent of self-assembling supramolecular dendrimer nanovectors holds great promise and heralds a new era of dendrimer-mediated delivery of RNA therapeutics in biomedical applications.

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Nanovaccines for remodeling the suppressive tumor microenvironment: New horizons in cancer immunotherapy
Kai Shi, Matthew Haynes, Leaf Huang
Front. Chem. Sci. Eng.. 2017, 11 (4): 676-684.   DOI: 10.1007/s11705-017-1640-4
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Despite limited successes in clinical development, therapeutic cancer vaccines have experienced resurgence in recent years due to an enhanced emphasis upon co-mitigating factors underlying immune response. Specifically, reversing the immune-suppressive effects of the tumor microenvironment, mediated by a variety of cellular and molecular signaling mechanisms, has become fundamental toward enhancing therapeutic efficacy. Therein, our lab has implemented various nano-vaccines based on the lipid-coated calcium phosphate platform for combined immunotherapy, in which antigenic, epitope-associated peptides as well as immune-suppression inhibitors can be co-delivered, often functioning through the same formulation. In probing the mechanism of action of such systems in vitro andin vivo, an improved effect synergy can be elucidated, inspiring future preclinical efforts and hope for clinical success.

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