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Nanopore containing graphene nanosheets were synthesized by graphene oxide and a reducing agent using a facile hydrothermal treatment in sodium hydroxide media. The as-prepared nanoporous graphene was incorporated into ethyl cellulose (EC) to prepare the mixed matrix membranes (MMMs) for C3H6/C3H8 separation. Transmission electron microscopy (TEM) photograph and X-ray photoelectron spectroscopy (XPS) analysis of nanoporous graphene nanosheets indicated that the structure of nano-pore was irregular and the oxygen-containing groups in the surface were limited. More importantly, the as-prepared MMMs presented better separation performance than that of pristine EC membrane due to simultaneous enhancement of C3H6 permeability and ideal selectivity. The ideal selectivity of the MMMs with 1.125 wt‰ nanoporous graphene content for C3H6/C3H8 increased from 3.45 to 10.42 and the permeability of C3H6 increased from 57.9 Barrer to 89.95 Barrer as compared with the pristine membrane. The presumed facilitated mechanism was that the high specific surface area of nanoporous graphene in polymer matrix increased the length of the tortuous pathway formed by nanopores for the gas diffusion as compared with the pristine graphene nanosheets, and generated a rigidified interface between the EC chains and fillers, thus enhanced the diffusivity selectivity. Therefore, it is expected that nanoporous graphene would be effective material for the C3H6/C3H8 separation.

The effect of tetracycline (TC) antibiotic on biogas generation in anaerobic wastewater treatment was studied. A lab-scale Anaerobic Baffled Reactor (ABR) with three compartments was used. The reactor was operated with synthetic wastewater in the absence of TC and in the presence of 250 μg/L TC for 90 days, respectively. The removal rate of TC, volatile fatty acids (VFAs), biogas compositions (hydrogen (H2), methane (CH4), carbon dioxide (CO2)), and total biogas production in each compartment were monitored in the two operational conditions. Results showed that the removal rate of TC was 14.97–67.97% in the reactor. The presence of TC had a large negative effect on CH4 and CO2 generation, but appeared to have a positive effect on H2 production and VFAs accumulation. This response indicated that the methanogenesis process was sensitive to TC presence, but the acidogenesis process was insensitive. This suggested that the presence of TC had less influence on the degradation of organic matter but had a strong influence on biogas generation. Additionally, the decrease of CH4 and CO2 generation and the increase of H2 and VFAs accumulation suggest a promising strategy to help alleviate global warming and improve resource recovery in an environmentally friendly approach.

High-solid anaerobic digestion is an attractive solution to the problem of sewage sludge disposal. One method that can be used to enhance the production of volatile fatty acids (VFAs) and the generation of methane from anaerobic digestion involves combining an alkaline pretreatment step with the synergistic effects of sewage sludge and cattle manure co-digestion, which improves the activity of key enzymes and microorganisms in the anaerobic co-digestion system to promote the digestion of organic waste. In this study, we describe an efficient strategy that involves adjusting the volatile solid (VS) ratio (sewage sludge/cattle manure: 3/7) and initial pH (9.0) to improve VFA production and methane generation from the co-digestion of sludge and manure. The experimental results indicate that the maximum VFA production was 98.33 g/kg-TS (total solid) at the optimal conditions. Furthermore, methane generation in a long-term semi-continuously operated reactor (at a VS ratio of 3/7 and pH of 9.0) was greater than 120.0 L/kg-TS.

Understanding the impact of all process parameters on the efficiency of biomass hydrolysis and on the final yield of products is critical to biorefinery design. Using Taguchi orthogonal arrays experimental design and Partial Least Square Regression, we investigated the impact of change and the comparative significance of thermochemical process temperature, treatment time, %Acid and %Solid load on carbohydrates release from green macroalgae from Ulva genus, a promising biorefinery feedstock. The average density of hydrolysate was determined using a new microelectromechanical optical resonator mass sensor. In addition, using Flux Balance Analysis techniques, we compared the potential fermentation yields of these hydrolysate products using metabolic models of Escherichia coli, Saccharomyces cerevisiae wild type, Saccharomyces cerevisiae RN1016 with xylose isomerase and Clostridium acetobutylicum. We found that %Acid plays the most significant role and treatment time the least significant role in affecting the monosaccharaides released from Ulva biomass. We also found that within the tested range of parameters, hydrolysis with 121 °C, 30 min 2% Acid, 15% Solids could lead to the highest yields of conversion: 54.134–57.500 gr ethanol kg−1Ulva dry weight by S. cerevisiae RN1016 with xylose isomerase. Our results support optimized marine algae utilization process design and will enable smart energy harvesting by thermochemical hydrolysis.

A new process consisting of a landfill bioreactor, partial-nitritation (PN) and the anammox process has been developed for landfill leachate treatment. In this study, the landfill bioreactor exhibited excellent performance in methane-rich biogas recovery, with a specific biogas yield of 0.47 L gas g−1 COD and methane percentages of 53–76%. PN was achieved in the aerobic reactor by high free ammonia (101 ± 83 mg NH3 L−1) inhibition for nitrite-oxidizing bacteria and the desired PN effluent composition (effluent nitrite: ammonium ratio of 1.1 ± 0.3) was controlled by adjusting the alkalinity concentration per unit of ammonium oxidized to approximately 14.3 mg CaCO3 mg−1 N in the influent. The startup of anammox process was successfully achieved with a membrane bioreactor in 160 d and a maximum nitrogen removal rate of 216 mg N L−1 d−1 was attained for real landfill leachate treatment. The quantitative polymerase chain reaction results confirmed that the cell-specific anammox activity was approximately 68–95 fmol N cell−1 d−1, which finally led to the stable operation of the system.

In this work it is shown how porous graphene aerogels fabricated by an eco-friendly and simple technological process, could be used as electrodes in lithium- ion batteries. The proposed graphene framework exhibited excellent performance including high reversible capacities, superior cycling stability and rate capability. A significantly lower temperature (75 °C) than the one currently utilized in battery manufacturing was utilized for self-assembly hence providing potential significant savings to the industrial production. After annealing at 600 °C, the formation of Sn-C-O bonds between the SnO2 nanoparticles and the reduced graphene sheets will initiate synergistic effect and improve the electrochemical performance. The XPS patterns revealed the formation of Sn-C-O bonds. Both SEM and TEM imaging of the electrode material showed that the three dimensional network of graphene aerogels and the SnO2 particles were distributed homogeneously on graphene sheets. Finally, the electrochemical properties of the samples as active anode materials for lithium-ion batteries were tested and examined by constant current charge–discharge cycling and the finding fully described in this manuscript.

Single-layered graphene has unique electronic, chemical, and electromechanical properties. Recently, graphite exfoliation in N-methylpyrrolidone and molten salt has been demonstrated to generate monolayer exfoliated graphene sheets (EGS). However, these solvents are either high-priced or require special care and have high boiling points and viscosities, making it difficult to deposit the dispersed graphene onto substrates. Here we show a universal principle for the exfoliation of graphite in water to single-layered and several-layered graphene sheets via the direct exfoliation of highly oriented pyrolytic graphite (HOPG) using pyridinium tribromide (Py(+)Br3(-)). Electrical conductivity5100 S/cm was observed for filtered graphene paper, and the EGS exhibited superior performance as a hole transport layer compared to the conventional material N,N-di(naphthalene-1-yl)-N,N-diphenylbenzidine at low voltage. The overall results demonstrate that this method is a scalable process for the preparation of highly conductive graphene for use in the commercial manufacture of high-performance electronic devices.

To enhance the treatment efficiency from an anaerobic digester, a novel six-compartment anaerobic/oxic baffled reactor (A/OBR) was employed. Two kinds of split-feeding A/OBRs R2 and R3, with influent fed in the 1st, 3rd and 5th compartment of the reactor simultaneously at the respective ratios of 6:3:1 and 6:2:2, were compared with the regular-feeding reactor R1 when all influent was fed in the 1st compartment (control). Three aspects, the COD removal, the hydraulic characteristics and the bacterial community, were systematically investigated, compared and evaluated. The results indicated that R2 and R3 had similar tolerance to loading shock, but the R2 had the highest COD removal of 91.6% with a final effluent of 345 mg/L. The mixing patterns in both split-feeding reactors were intermediate between plug-flow and completely-mixed, with dead spaces between 8.17% and 8.35% compared with a 31.9% dead space in R1. Polymerase chain reaction-denaturing gradient gel electrophoresis (PCR-DGGE) analysis revealed that the split-feeding strategy provided a higher bacterial diversity and more stable bacterial community than that in the regular-feeding strategy. Further analysis indicated that Firmicutes, Bacteroidetes, and Proteobacteria were the dominant bacteria, among which Firmicutes and Bacteroidetes might be responsible for organic matter degradation and Proteobacteria for nitrification and denitrification.

MFC centered hybrid technologies have attracted attention during the last few years due to their compatibility and dual advantages of energy recovery and wastewater treatment. In this study, a MFC was integrated into a dewatered alum sludge (DAS)- based vertical upflow constructed wetland (CW). Powder activate carbon (PAC) was used in the anode area in varied percentage with DAS to explore its influences on the performance of the CW-MFC system. The trial has demonstrated that the inclusion of PAC improved the removal efficiencies of COD, TN and RP. More significantly, increasing the proportion of PAC from 2% to 10% can significantly enhance the maximum power densities from 36.58 mW/m2 to 87.79 mW/m2. The induced favorable environment for bio-cathode formation might be the main reason for this improvement since the content of total extracellular polymeric substances (TEPS) of the substrate in the cathode area almost doubled (from 44.59 μg/g wet sludge to 87.70 μg/g wet sludge) as the percentage of PAC increased to 10%. This work provides another potential usage of PAC in CW-MFCs with a higher wastewater treatment efficiency and energy recovery.

Nitrogen-doped (N-doped) graphene has been prepared by a simple one-step hydrothermal approach using hexamethylenetetramine (HMTA) as single carbon and nitrogen source. In this hydrothermal process, HMTA pyrolyzes at high temperature and the N-doped graphene subsequently self-assembles on the surface of MgO particles (formed by the Mg powder reacting with H2O) during which graphene synthesis and nitrogen doping are simultaneously achieved. The as-synthesized graphene with incorporation of nitrogen groups possesses unique structure including thin layer thickness, high surface area, mesopores and vacancies. These structural features and their synergistic effects could not only improve ions and electrons transportation with nanometer-scale diffusion distances but also promote the penetration of electrolyte. The N-doped graphene exhibits high reversible capacity, superior rate capability as well as long-term cycling stability, which demonstrate that the N-doped graphene with great potential to be an efficient electrode material. The experimental results provide a new hydrothermal route to synthesize N-doped graphene with potential application for advanced energy storage, as well as useful information to design new graphene materials.

Hsieh, MC., Koga, H., Suganuma, K. et al. Hazy Transparent Cellulose Nanopaper. Sci Rep 7, 41590 (2017). https://doi.org/10.1038/srep41590., The aim of this study is to clarify light scattering mechanism of hazy transparent cellulose nanopaper. Clear optical transparent nanopaper consists of 3-15 nm wide cellulose nanofibers, which are obtained by the full nanofibrillation of pulp fibers. At the clear transparent nanopaper with 40 μm thickness, their total transmittance are 89.3-91.5% and haze values are 4.9-11.7%. When the pulp fibers are subjected to weak nanofibrillation, hazy transparent nanopapers are obtained. The hazy transparent nanopaper consists of cellulose nanofibers and some microsized cellulose fibers. At the hazy transparent nanopaper with 40 μm thickness, their total transmittance were constant at 88.6-92.1% but their haze value were 27.3-86.7%. Cellulose nanofibers are solid cylinders, whereas the pulp fibers are hollow cylinders. The hollow shape is retained in the microsized cellulose fibers, but they are compressed flat inside the nanopaper. This compressed cavity causes light scattering by the refractive index difference between air and cellulose. As a result, the nanopaper shows a hazy transparent appearance and exhibits a high thermal durability (295-305 °C), and low thermal expansion (8.5-10.6 ppm/K) because of their high density (1.29-1.55 g/cm3) and crystallinity (73-80%).

To pattern electrical metal contacts, electron beam lithography or photolithography are commonly utilized and these processes require polymer resists with solvents. During the patterning process the graphene surface is exposed to chemicals and the residue on the graphene surface was unable to be completely removed by any method, causing the graphene layer to be contaminated. A lithography free method can overcome these residue problems. In this study, we use a micro-grid as a shadow mask to fabricate a graphene based field-effect-transistor (FET). Electrical measurements of the graphene based FET samples are carried out in air and vacuum. It is found that the Dirac peaks of the graphene devices on SiO2 or on hexagonal boron nitride (hBN) shift from a positive gate voltage region to a negative region as air pressure decreases. In particular, the Dirac peaks shift very rapidly when the pressure decreases from ~2 × 10−3 Torr to ~5 × 10−5 Torr within 5 minutes. These Dirac peak shifts are known as adsorption and desorption of environmental gases, but the shift amounts are considerably different depending on the fabrication process. The high gas sensitivity of the device fabricated by shadow mask is attributed to adsorption on the clean graphene surface.

Ethanol fermentation requires oxygen to maintain high biomass and cell viability, especially under very-high-gravity (VHG) condition. In this work, fermentation redox potential (ORP) was applied to drive the aeration process at low dissolved oxygen (DO) levels, which is infeasible to be regulated by a DO sensor. The performance and characteristics of flocculating yeast grown under 300 and 260 g glucose/L conditions were subjected to various aeration strategies including: no aeration; controlled aeration at −150, −100 and −50 mV levels; and constant aeration at 0.05 and 0.2 vvm. The results showed that anaerobic fermentation produced the least ethanol and had the highest residual glucose after 72 h of fermentation. Controlled aerations, depending on the real-time oxygen demand, led to higher cell viability than the no-aeration counterpart. Constant aeration triggered a quick biomass formation, and fast glucose utilization. However, over aeration at 0.2 vvm caused a reduction of final ethanol concentration. The controlled aeration driven by ORP under VHG conditions resulted in the best fermentation performance. Moreover, the controlled aeration could enhance yeast flocculating activity, promote an increase of flocs size, and accelerate yeast separation near the end of fermentation.

Stable nitritation is a critical bottleneck for achieving autotrophic nitrogen removal using the energy-saving mainstream deammonification process. Herein we report a new strategy to wash out both the Nitrospira sp. and Nitrobacter sp. from the treatment of domestic-strength wastewater. The strategy combines sludge treatment using free nitrous acid (FNA) with dissolved oxygen (DO) control in the nitritation reactor. Initially, the nitrifying reactor achieved full conversion of NH4+ to NO3−. Then, nitrite accumulation at ~60% was achieved in the reactor when 1/4 of the sludge was treated daily with FNA at 1.82 mg N/L in a side-stream unit for 24 h. Fluorescence in-situ hybridization (FISH) revealed FNA treatment substantially reduced the abundance of nitrite oxidizing bacteria (NOB) (from 23.0 ± 4.3 to 5.3 ± 1.9%), especially that of Nitrospira sp. (from 15.7 ± 3.9 to 0.4 ± 0.1%). Nitrite accumulation increased to ~80% when the DO concentration in the mainstream reactor was reduced from 2.5–3.0 to 0.3–0.8 mg/L. FISH revealed the DO limitation further reduced the abundance of NOB (to 2.1 ± 1.0%), especially that of Nitrobacter sp. (from 4.9 ± 1.2 to 1.8 ± 0.8%). The strategy developed removes a major barrier for deammonification in low-strength domestic wastewater.

Although graphene is a typical two dimensional materials, it has converted to multi-dimensional materials with many unique properties. As an example, the one dimensional graphene fiber is fabricated by utilizing ionic liquid as coagulation and functional diamines as cross-linkers to connect graphene oxide layers. The fibers show excellent mechanical properties and superior electrical performance. The tensile strength of the resultant fibers reaches ~729 MPa after a super high temperature thermal annealing treatment at 2800 °C. Additionally, quasi-solid-state flexible micro-capacitors are fabricated with promising result on energy storage. The device show a specific volumetric capacity as high as ~225 F/cm3 (measured at 103.5 mA cm−3 in a three-electrode cell), as well as a long cycle life of 2000 times. The initial results indicate that these fibers will be a good candidate to replace energy storage devices for miniaturized portable electronic applications.

To meet the high quality standard of receiving water, the coagulation process using polyferric chloride (PFC) was used to further improve the water quality of effluent from wastewater treatment plants. Uniform design (UD) coupled with response surface methodology (RSM) was adopted to assess the effects of the main influence factors: coagulant dosage, pH and basicity, on the removal of total organic carbon (TOC), NH4+-N and PO43−-P. A desirability function approach was used to effectively optimize the coagulation process for the comprehensive removal of TOC, NH4+-N and PO43−-P to upgrade the effluent quality in practical application. The optimized operating conditions were: dosage 28 mg/L, pH 8.5 and basicity 0.001. The corresponding removal efficiencies for TOC, NH4+-N and PO43−-P were 77.2%, 94.6% and 20.8%, respectively. More importantly, the effluent quality could upgrade to surface water Class V of China through coagulation under optimal region. In addition, grey relational analysis (GRA) prioritized these three factors as: pH > basicity > dosage (for TOC), basicity > dosage > pH (for NH4+-N), pH > dosage > basicity (for PO43−-P), which would help identify the most important factor to control the treatment efficiency of various effluent quality indexes by PFC coagulation.

The utilization of bioethanol as the alcohol source for biodiesel production is more environmentally advantageous over methanol owing to its lower toxicity, lower flammability and its sustainable supply from renewable agricultural resources. However, as the presence of water in crude bioethanol is the critical factor limiting the biodiesel production process, the energy-intensive and costly purification of bioethanol is necessary for biodiesel application. Manganese glycerolate (MnGly) is reported the first time here as a robust heterogeneous catalyst that exhibited over 90% conversion by using aqueous ethanol containing 80 wt.% of water in the production of fatty acid ethyl ester (FAEE). The employment of 95 wt.% ethanol with respect to water could achieve 99.7% feedstock conversion in 6 hours under the optimal reaction conditions: reaction temperature (150 °C), feedstock-to-ethanol molar ratio (1:20) and catalyst loading (6 wt.%). Commercially available low grade crude bioethanol with the presence of impurities like sugars were applied which demonstrated remarkable catalytic activity in 24 hours. The high water tolerance of MnGly towards biodiesel production could eventually simplify the purification of bioethanol that consumes less energy and production cost.

The increasing demand of emerging technologies for high energy density electrochemical storage has led many researchers to look for alternative anode materials to graphite. The most promising conversion and alloying materials do not yet possess acceptable cycle life or rate capability. In this work, we use tin oxide, SnO2, as a representative anode material to explore the influence of graphene incorporation and In-doping to increase the electronic conductivity and concomitantly improve capacity retention and cycle life. It was found that the incorporation of In into SnO2 reduces the charge transfer resistance during cycling, prolonging life. It is also hypothesized that the increased conductivity allows the tin oxide conversion and alloying reactions to both be reversible, leading to very high capacity near 1200 mAh/g. Finally, the electrodes show excellent rate capability with a capacity of over 200 mAh/g at 10C.

A novel biological nitrogen removal system based on nitritation coupled with thiosulfate-driven denitritation (Nitritation-TDD) was developed to achieve a high nitrogen removal rate and low sludge production. A nitritation sequential batch reactor (nitritation SBR) and an anoxic up-flow sludge bed (AnUSB) reactor were applied for effective nitritation and denitritation, respectively. Above 75% nitrite was accumulated in the nitritation SBR with an influent ammonia loading rate of 0.43 kg N/d/m3. During Nitritation-TDD operation, particle sizes (d50) of the sludge decreased from 406 to 225 um in nitritation SBR and from 327–183 um in AnUSB reactor. Pyrosequencing tests revealed that ammonium-oxidizing bacteria (AOB) population was stabilized at approximately 7.0% (calculated as population of AOB-related genus divided by the total microbial population) in the nitritation SBR. In contrast, nitrite-oxidizing bacteria (NOB) population decreased from 6.5–0.6% over the same time, indicating the effective nitrite accumulation in the nitritation SBR. Thiobacillus, accounting for 34.2% in the AnUSB reactor, was mainly responsible for nitrogen removal via autotrophic denitritation, using an external source of thiosulfate as electron donor. Also, it was found that free nitrous acid could directly affect the denitritation activity.

Understanding the underlying mechanisms involved in graphene growth via chemical vapour deposition (CVD) is critical for precise control of the characteristics of graphene. Despite much effort, the actual processes behind graphene synthesis still remain to be elucidated in a large number of aspects. Herein, we report the evolution of graphene properties during in-plane growth of graphene from reduced graphene oxide (RGO) on copper (Cu) via methane CVD. While graphene is laterally grown from RGO flakes on Cu foils up to a few hundred nanometres during CVD process, it shows appreciable improvement in structural quality. The monotonous enhancement of the structural quality of the graphene with increasing length of the graphene growth from RGO suggests that seeded CVD growth of graphene from RGO on Cu surface is accompanied by the restoration of graphitic structure. The finding provides insight into graphene growth and defect reconstruction useful for the production of tailored carbon nanostructures with required properties.

Porous structure of reduced graphene oxide (rGO) plays an important role in developing flexible graphene-based devices. In this work, we report a novel methodology for reduction of freestanding graphite oxide (GO) sheet by picosecond pulse laser direct writing in liquid nitrogen. Non-agglomerate and porous structure of rGO is fabricated successfully due to frozen effect during laser processing. Compared with laser-irradiated rGO developed in N2 gas at ambient environment, the frozen rGO developed in liquid N2 shows better ordered structure with less defects, crack-free morphology as well as better electron supercapacitor performance including 50–60 Ω/sq in sheet electrical resistance. Mechanism of cryotemperature photoreduction GO is also discussed.

In this work, a novel platform for surface-enhanced Raman spectroscopy (SERS)-based chemical sensors utilizing three-dimensional microporous graphene foam (GF) decorated with silver nanoparticles (AgNPs) is developed and applied for methylene blue (MB) detection. The results demonstrate that silver nanoparticles significantly enhance cascaded amplification of SERS effect on multilayer graphene foam (GF). The enhancement factor of AgNPs/GF sensor is found to be four orders of magnitude larger than that of AgNPs/Si substrate. In addition, the sensitivity of the sensor could be tuned by controlling the size of silver nanoparticles. The highest SERS enhancement factor of ∼5 × 104 is achieved at the optimal nanoparticle size of 50 nm. Moreover, the sensor is capable of detecting MB over broad concentration ranges from 1 nM to 100 μM. Therefore, AgNPs/GF is a highly promising SERS substrate for detection of chemical substances with ultra-low concentrations.

Recovery of nutrients and energy from municipal wastewater has attracted much attention in recent years; however, its efficiency is significantly limited by the low-strength properties of municipal wastewater. Herein, we report a pilot-scale forward osmosis (FO) system using a spiral-wound membrane module to concentrate real municipal wastewater. Under active layer facing feed solution mode, the critical concentration factor (CCF) of this FO system was determined to be 8 with 0.5 M NaCl as draw solution. During long-term operation at a concentration factor of 5, (99.8 ± 0.6)% of chemical oxygen demand and (99.7 ± 0.5)% of total phosphorus rejection rates could be achieved at a flux of 6 L/(m2 h) on average. In comparison, only (48.1 ± 10.5)% and (67.8 ± 7.3)% rejection of ammonium and total nitrogen were observed. Cake enhanced concentration polarization is a major contributor to the decrease of water fluxes. The fouling also led to the occurrence of a cake reduced concentration polarization effect, improving ammonium rejection rate with the increase of operation time in each cycle. This work demonstrates the applicability of using FO process for wastewater concentrating and also limitations in ammonium recovery that need further improvement in future.

The successful integration of graphene into microelectronic devices is strongly dependent on the availability of direct deposition processes, which can provide uniform, large area and high quality graphene on nonmetallic substrates. As of today the dominant technology is based on Si and obtaining graphene with Si is treated as the most advantageous solution. However, the formation of carbide during the growth process makes manufacturing graphene on Si wafers extremely challenging. To overcome these difficulties and reach the set goals, we proposed growth of high quality graphene layers by the CVD method on Ge(100)/Si(100) wafers. In addition, a stochastic model was applied in order to describe the graphene growth process on the Ge(100)/Si(100) substrate and to determine the direction of further processes. As a result, high quality graphene was grown, which was proved by Raman spectroscopy results, showing uniform monolayer films with FWHM of the 2D band of 32 cm−1.

Cellulosic ethanol production from lignocellulosic biomass offers a sustainable solution for transition from fossil based fuels to renewable alternatives. However, a few long-standing technical challenges remain to be addressed in the development of an economically viable fermentation process from lignocellulose. Such challenges include the needs to improve yeast tolerance to toxic inhibitory compounds and to achieve high fermentation efficiency with minimum detoxification steps after a simple biomass pretreatment. Here we report an in-situ detoxification strategy by PEG exo-protection of an industrial dry yeast (starch-base). The exo-protected yeast cells displayed remarkably boosted vitality with high tolerance to toxic inhibitory compounds and with largely improved ethanol productivity from crude hydrolysate derived from a pretreated lignocellulose. The PEG chemical exo-protection makes the industrial S. cerevisiae yeast directly applicable for the production of cellulosic ethanol with substantially improved productivity and yield, without of the need to use genetically modified microorganisms.

Anaerobic digestion (AD) plays an important role in waste activated sludge (WAS) treatment; however, conventional AD (CAD) process needs substantial improvements, especially for the treatment of WAS with low solids content and poor anaerobic biodegradability. Herein, we propose a submerged anaerobic dynamic membrane bioreactor (AnDMBR) for simultaneous WAS thickening and digestion without any pretreatment. During the long-term operation, the AnDMBR exhibited an enhanced sludge reduction and improved methane production over CAD process. Moreover, the biogas generated in the AnDMBR contained higher methane content than CAD process. Stable carbon isotopic signatures elucidated the occurrence of combined methanogenic pathways in the AnDMBR process, in which hydrogenotrophic methanogenic pathway made a larger contribution to the total methane production. It was also found that organic matter degradation was enhanced in the AnDMBR, thus providing more favorable substrates for microorganisms. Pyrosequencing revealed that Proteobacteria and Bacteroidetes were abundant in bacterial communities and Methanosarcina and Methanosaeta in archaeal communities, which played an important role in the AnDMBR system. This study shed light on the enhanced digestion of WAS using AnDMBR technology.

Iron oxide nanoparticles (NPs) are considered as an attractive energy storage and catalyst material due to high theoretical lithium capacity, good (electro)catalytic activity, environmental friendliness, high abundance, and low cost1,2. In order to manipulate physical and electrochemical properties, diverse nanostructures of iron oxide NPs such as porous particle3, 0D nanoparticle4,5, 1D nanowires and nanotubes6,7,8, 2D nanoflakes and nanosheet9,10, and 3D flowerlike and hollow structures11,12 have been developed for applications into lithium ion battery (LIB) anode and photocatalysis. Along with the nanoscale architecturing, the crystalline phases (e.g. hematite, maghemite and magnetite) and oxidation states (e.g. Fe2+ and Fe3+) of iron oxide need to be delicately controlled for achieving desirable properties and for adapting functionality13. Despite these features originating from structure and crystalline phase, iron oxide NP itself as a single component has its own limitations. For instance, iron oxide NPs obtain the shortcomings of low electronic conductivity and electrode pulverization when they electrochemically store lithium ions1, thereby revealing limited rate and cyclic performances. Furthermore, photo-Fenton reaction using iron oxides, which is very useful for the degradation or mineralization of harmful/toxic pollutants in water and wastewater, demonstrated the drawbacks of poor recycling and low catalyst stability6. Accordingly, much effort has been devoted to resolve the afore-mentioned challenges by nanostructuring and hybridization1,13. Recently, the integration of metal oxide (MO) active materials with the conductive carbon matrices has gained significant attention as an emerging class of functional hybrid materials owing to the appealing electrochemical properties, large surface area, and chemical and mechanical stabilities of carbon nanomaterials for energy storage and catalytic applications14,15. Various iron oxide/carbon nanocomposites such as 1D iron oxide/carbon nanowires16, 2D iron oxide/carbon hybrid nanosheets17, and 3D iron oxide/carbon nanostructures18 have been developed for improving the electrochemical and catalytic properties of iron oxide. In particular, hierarchical architecturing of graphene/MO hybrids in a three-dimensional (3D) manner is expected to become an innovative chemical approach for full potential of respective functionality. In addition to intrinsic material properties, such a hierarchical structure constructed by graphene nanosheets and MO NPs takes advantages of 3D interconnected macroscopic structure in terms of a large accessible area, fast mass and ion transport, percolated charge transfer, and structural integrity19,20,21. For instance, Ma et al. demonstrated one-step, solvothermal synthesis of 3D self-assembled reduced graphene oxide (rGO)/CoO hybrids22. Wu et al. reported 3D graphene aerogel/Fe3O4 hybrids for electrocatalysis23. However, neither the synthetic method was environmentally benign nor multi-functionality of as-obtained hybrid was demonstrated. Accordingly, it is important to develop the one-pot synthesis of hierarchically structured graphene/MO nanohybrids through solution chemistry and subsequent phase control of iron oxide NPs for specific applications. Herein, we demonstrate the one-pot, hydrothermal synthesis of hierarchically structured rGO/α-Fe2O3 and rGO/γ-Fe3O4 nanobox hybrids (hrGO/α-Fe and hrGO/γ-Fe NBhs) for LIB anodes and photo-Fenton catalysis. All in one synthetic approach is very simple yet useful for simultaneously constructing 3D macroscopic rGO structures and growing α-Fe2O3 NBs. Even after the subsequent reduction from α-Fe2O3 into γ-Fe3O4, hierarchical architectures remained intact. These hrGO/Fe NBhs showed excellent battery and photocatalytic performances.

A heat-initiated chemical reaction was developed to functionalize CVD-grown graphene at wafer scale and the reaction was universally extended to carbon nanotubes and other precursors that could be thermally converted to active radicals. The chemical reaction can occur in absence of oxygen and water vapor when the temperature is above the decomposition temperature of the reactants. The chemical reaction was also found to be substrate-dependent due to surface doping and inhomogeneity. A large-scale graphene pattern was demonstrated by combing with microfluidic technique. This heat-initiated solid-phase chemical reaction provides a facile and environmentally friendly approach to functionalize carbon nanomaterials with various functional groups.

A continuous stirred microbial electrochemical reactor (CSMER), comprising of a complete mixing zone (CMZ) and microbial electrochemical zone (MEZ), was used for brewery wastewater treatment. The system realized 75.4 ± 5.7% of TCOD and 64.9 ± 4.9% of TSS when fed with brewery wastewater concomitantly achieving an average maximum power density of 304 ± 31 m W m−2. Cascade utilization of organic matters made the CSMER remove a wider range of substrates compared with a continuous stirred tank reactor (CSTR), in which process 79.1 ± 5.6% of soluble protein and 86.6 ± 2.2% of soluble carbohydrates were degraded by anaerobic digestion in the CMZ and short-chain volatile fatty acids were further decomposed and generated current in the MEZ. Co-existence of fermentative bacteria (Clostridium and Bacteroides, 19.7% and 5.0%), acetogenic bacteria (Syntrophobacter, 20.8%), methanogenic archaea (Methanosaeta and Methanobacterium, 40.3% and 38.4%) and exoelectrogens (Geobacter, 12.4%) as well as a clear spatial distribution and syntrophic interaction among them contributed to the cascade degradation process in CSMER. The CSMER shows great promise for practical wastewater treatment application due to high pre-hydrolysis and acidification rate, high energy recovery and low capital cost.

Single-layer graphene has demonstrated remarkable electronic properties that are strongly influenced by interfacial bonding and break down for the lowest energy configuration of stacked graphene layers (AB Bernal). Multilayer graphene with relative rotations between carbon layers, known as turbostratic graphene, can effectively decouple the electronic states of adjacent layers, preserving properties similar to that of SLG. While the growth of AB Bernal graphene through chemical vapor deposition has been widely reported, we investigate the growth of turbostratic graphene on heteroepitaxial Ni(111) thin films utilizing physical vapor deposition. By varying the carbon deposition temperature between 800 –1100 °C, we report an increase in the graphene quality concomitant with a transition in the size of uniform thickness graphene, ranging from nanocrystallites to thousands of square microns. Combination Raman modes of as-grown graphene within the frequency range of 1650 cm−1 to 2300 cm−1, along with features of the Raman 2D mode, were employed as signatures of turbostratic graphene. Bilayer and multilayer graphene were directly identified from areas that exhibited Raman characteristics of turbostratic graphene using high-resolution TEM imaging. Raman maps of the pertinent modes reveal large regions of turbostratic graphene on Ni(111) thin films at a deposition temperature of 1100 °C.

Green chemistry, sustainability and eco-efficiency are guiding the development of the next generation of industrial chemical processes. The use of non-edible lignocellulosic biomass as a source of chemicals and fuels has recently raised interest due to the need for an alternative to fossil resources. Valorisation mainly focuses on cellulose, which has been used for various industrial scale applications for decades. However, creating an economically more viable value chain would require the exploitation of the other main components, hemicellulose and lignin. Here, we present a new low melting mixture composition based in boric acid and choline chloride and demonstrate its efficiency in the fractionation of wood-based biomass for the production of non-condensed lignin, suitable for further use in the search for sustainable industrial applications and for the selective conversion of hemicelluloses into valuable platform chemicals.

A new self-assembly concept is introduced to form large and pristine films (15 cm in diameter) of reduced graphene oxide (RGO). The resulting film has different degrees of polarity on its two different sides due to the characteristic nature of the self-assembly process. The RGO film can be easily transferred from a glass substrate onto water and a polymer substrate after injection of water molecules between the RGO film and glass substrate using an electric steamer. The RGO film can also be easily patterned into various shapes with a resolution of around ±10 μm by a simple taping method, which is suitable for mass production of printed electronics at low cost.

Energy self-sufficiency is a highly desirable goal of sustainable wastewater treatment. Herein, a combined system of a microbial fuel cell and an intermittently aerated biological filter (MFC-IABF) was designed and operated in an energy self-sufficient manner. The system was fed with synthetic wastewater (COD = 1000 mg L−1) in continuous mode for more than 3 months at room temperature (~25 °C). Voltage output was increased to 5 ± 0.4 V using a capacitor-based circuit. The MFC produced electricity to power the pumping and aeration systems in IABF, concomitantly removing COD. The IABF operating under an intermittent aeration mode (aeration rate 1000 ± 80 mL h−1) removed the residual nutrients and improved the water quality at HRT = 7.2 h. This two-stage combined system obtained 93.9% SCOD removal and 91.7% TCOD removal (effluent SCOD = 61 mg L−1, TCOD = 82.8 mg L−1). Energy analysis indicated that the MFC unit produced sufficient energy (0.27 kWh m−3) to support the pumping system (0.014 kWh m−3) and aeration system (0.22 kWh m−3). These results demonstrated that the combined MFC-IABF system could be operated in an energy self-sufficient manner, resulting to high-quality effluent.

There is significant interest in synthesizing large-area graphene films at low temperatures by chemical vapor deposition (CVD) for nanoelectronic and flexible device applications. However, to date, low-temperature CVD methods have suffered from lower surface coverage because micro-sized graphene flakes are produced. Here, we demonstrate a modified CVD technique for the production of large-area, continuous monolayer graphene films from benzene on Cu at 100–300 °C at ambient pressure. In this method, we extended the graphene growth step in the absence of residual oxidizing species by introducing pumping and purging cycles prior to growth. This led to continuous monolayer graphene films with full surface coverage and excellent quality, which were comparable to those achieved with high-temperature CVD; for example, the surface coverage, transmittance and carrier mobilities of the graphene grown at 300 °C were 100%, 97.6% and 1,900–2,500 cm2 V−1 s−1, respectively. In addition, the growth temperature was substantially reduced to as low as 100 °C, which is the lowest temperature reported to date for pristine graphene produced by CVD. Our modified CVD method is expected to allow the direct growth of graphene in device manufacturing processes for practical applications while keeping underlying devices intact.

This study presents a simple and sustainable Microbial Fuel Cell as a standalone, self-powered reactor for in situ wastewater electrolysis, recovering nitrogen from wastewater. A process is proposed whereby the MFC electrical performance drives the electrolysis of wastewater towards the self-generation of catholyte within the same reactor. The MFCs were designed to harvest the generated catholyte in the internal chamber, which showed that liquid production rates are largely proportional to electrical current generation. The catholyte demonstrated bactericidal properties, compared to the control (open-circuit) diffusate and reduced observable biofilm formation on the cathode electrode. Killing effects were confirmed using bacterial kill curves constructed by exposing a bioluminescent Escherichia coli target, as a surrogate coliform, to catholyte where a rapid kill rate was observed. Therefore, MFCs could serve as a water recovery system, a disinfectant/cleaner generator that limits undesired biofilm formation and as a washing agent in waterless urinals to improve sanitation. This simple and ready to implement MFC system can convert organic waste directly into electricity and self-driven nitrogen along with water recovery. This could lead to the development of energy positive bioprocesses for sustainable wastewater treatment.

Graphene has recently attracted much interest as a material for flexible, transparent electrodes or active layers in electronic and photonic devices. However, realization of such graphene-based devices is limited due to difficulties in obtaining patterned graphene monolayers on top of materials that are degraded when exposed to a high-temperature or wet process. We demonstrate a low-temperature, dry process capable of transfer-printing a patterned graphene monolayer grown on Cu foil onto a target substrate using an elastomeric stamp. A challenge in realizing this is to obtain a high-quality graphene layer on a hydrophobic stamp made of poly(dimethylsiloxane), which is overcome by introducing two crucial modifications to the conventional wet-transfer method – the use of a support layer composed of Au and the decrease in surface tension of the liquid bath. Using this technique, patterns of a graphene monolayer were transfer-printed on poly(3,4-ethylenedioxythiophene):polystyrene sulfonate and MoO3, both of which are easily degraded when exposed to an aqueous or aggressive patterning process. We discuss the range of application of this technique, which is currently limited by oligomer contaminants and possible means to expand it by eliminating the contamination problem.

We developed a simple, scalable and high-throughput method for fabrication of large-area three-dimensional rose-like microflowers with controlled size, shape and density on graphene films by femtosecond laser micromachining. The novel biomimetic microflower that composed of numerous turnup graphene nanoflakes can be fabricated by only a single femtosecond laser pulse, which is efficient enough for large-area patterning. The graphene films were composed of layer-by-layer graphene nanosheets separated by nanogaps (~10–50 nm) and graphene monolayers with an interlayer spacing of ~0.37 nm constituted each of the graphene nanosheets. This unique hierarchical layering structure of graphene films provides great possibilities for generation of tensile stress during femtosecond laser ablation to roll up the nanoflakes, which contributes to the formation of microflowers. By a simple scanning technique, patterned surfaces with controllable densities of flower patterns were obtained, which can exhibit adhesive superhydrophobicity. More importantly, this technique enables fabrication of the large-area patterned surfaces at centimeter scales in a simple and efficient way. This study not only presents new insights of ultrafast laser processing of novel graphene-based materials but also shows great promise of designing new materials combined with ultrafast laser surface patterning for future applications in functional coatings, sensors, actuators and microfluidics.

We introduce a real-time method to monitor the evolution of oak aromas during the oak toasting process. French and American oak wood boards were toasted in an oven at three different temperatures, while the process-gas was continuously transferred to the inlet of a proton-transfer-reaction time-of-flight mass spectrometer for online monitoring. Oak wood aroma compounds important for their sensory contribution to oak-aged wine were tentatively identified based on soft ionization and molecular mass. The time-intensity profiles revealed toasting process dynamics illustrating in real-time how different compounds evolve from the oak wood during toasting. Sufficient sensitivity was achieved to observe spikes in volatile concentrations related to cracking phenomena on the oak wood surface. The polysaccharide-derived compounds exhibited similar profiles; whilst for lignin-derived compounds eugenol formation differed from that of vanillin and guaiacol at lower toasting temperatures. Significant generation of oak lactone from precursors was evident at 225 oC. Statistical processing of the real-time aroma data showed similarities and differences between individual oak boards and oak wood sourced from the different origins. This study enriches our understanding of the oak toasting process and demonstrates a new analytical approach for research on wood volatiles.

The efficiency of flexible photovoltaic and organic light emitting devices is heavily dependent on the availability of flexible and transparent conductors with at least a similar workfunction to that of Indium Tin Oxide. Here we present the first study of the work function of large area (up to 9 cm2) FeCl3 intercalated graphene grown by chemical vapour deposition on Nickel and demonstrate values as large as 5.1 eV. Upon intercalation, a charge density per graphene layer of 5 ⋅ 1013 ± 5 ⋅ 1012 cm−2 is attained, making this material an attractive platform for the study of plasmonic excitations in the infrared wavelength spectrum of interest to the telecommunication industry. Finally, we demonstrate the potential of this material for flexible electronics in a transparent circuit on a polyethylene naphthalate substrate.

This study reports a scalable and economical method to open a band gap in single layer graphene by deposition of cobalt metal on its surface using physical vapor deposition in high vacuum. At low cobalt thickness, clusters form at impurity sites on the graphene without etching or damaging the graphene. When exposed to oxygen at room temperature, oxygen functional groups form in proportion to the cobalt thickness that modify the graphene band structure. Cobalt/Graphene resulting from this treatment can support a band gap of 0.30 eV, while remaining largely undamaged to preserve its structural and electrical properties. A mechanism of cobalt-mediated band opening is proposed as a two-step process starting with charge transfer from metal to graphene, followed by formation of oxides where cobalt has been deposited. Contributions from the formation of both CoO and oxygen functional groups on graphene affect the electronic structure to open a band gap. This study demonstrates that cobalt-mediated oxidation is a viable method to introduce a band gap into graphene at room temperature that could be applicable in electronics applications.

Composting is a widely-used method to recycle the nutrients in livestock manure for agriculture. The spatial stratifications of microbial processes inside the manure particle that determine organic and nitrogen transformation are virtually unclear. Here, we show the evolution of the interior microenvironment of swine, cow and chicken manure by using microelectrodes during forced-aeration composting. Composting has generally been regarded as an aerobic bioprocess, however, the long-existing of a large anoxic zone inside these manures was confirmed during the active phase in this study. The profile of the oxidation–reduction potential dramatically decreased first and then gradually increased. The spatial difference in the ammonia concentration was not significant, but nitrate concentration continuously decreased with depth. The anoxic condition within the manure particle was demonstrated to be a primary cause of the severe ammonia emission and the long composting period. These founding provided a new insight toward “aerobic” composting process and a sound foundation for the development of efficient composting technology.

Biological wastewater treatment processes under a dynamic regime with respect to carbon substrate can result in microbial storage of internal polymers (e.g., polyhydroxybutyrate (PHB)) and their subsequent utilizations. These storage turnovers play important roles in nitrous oxide (N2O) accumulation during heterotrophic denitrification in biological wastewater treatment. In this work, a mathematical model is developed to evaluate the key role of PHB storage turnovers on N2O accumulation during denitrification for the first time, aiming to establish the key relationship between N2O accumulation and PHB storage production. The model is successfully calibrated and validated using N2O data from two independent experimental systems with PHB storage turnovers. The model satisfactorily describes nitrogen reductions, PHB storage/utilization and N2O accumulation from both systems. The results reveal a linear relationship between N2O accumulation and PHB production, suggesting a substantial effect of PHB storage on N2O accumulation during denitrification. Application of the model to simulate long-term operations of a denitrifying sequencing batch reactor and a denitrifying continuous system indicates the feeding pattern and sludge retention time would alter PHB turnovers and thus affect N2O accumulation. Increasing PHB utilization could substantially raise N2O accumulation due to the relatively low N2O reduction rate when using PHB as carbon source.

Graphene/Cu composites were fabricated through a graphene in-situ grown approach, which involved ball-milling of Cu powders with PMMA as solid carbon source, in-situ growth of graphene on flaky Cu powders and vacuum hot-press sintering. SEM and TEM characterization results indicated that graphene in-situ grown on Cu powders guaranteed a homogeneous dispersion and a good combination between graphene and Cu matrix, as well as the intact structure of graphene, which was beneficial to its strengthening effect. The yield strength of 244 MPa and tensile strength of 274 MPa were achieved in the composite with 0.95 wt.% graphene, which were separately 177% and 27.4% enhancement over pure Cu. Strengthening effect of in-situ grown graphene in the matrix was contributed to load transfer and dislocation strengthening.

Modification of titanium dioxide (TiO2) for H2 generation is a grand challenge due to its high chemical inertness, large bandgap, narrow light-response range and rapid recombination of electrons and holes. Herein, we report a simple process to prepare nanospherical like reduced graphene oxide (NS-rGO) decorated TiO2 nanoparticles (NS-rGO/TiO2) as photocatalysts. This modified TiO2 sample exhibits remarkably significant improvement on visible light absorption, narrow band gap and efficient charge collection and separation. The photocatalytic H2 production rate of NS-rGO/TiO2 is high as 13996 μmol g−1 h−1, which exceeds that obtained on TiO2 alone and TiO2 with parallel graphene sheets by 3.45 and 3.05 times, respectively. This improvement is due to the presence of NS-rGO as an electron collector and transporter. The geometry of NS-rGO should be effective in the design of a graphene/TiO2 composite for photocatalytic applications.

We report a detailed investigation of the structural and chemical characteristics of thin evaporated Al2O3 tunnel barriers of variable thickness grown onto single-layer graphene sheets. Advanced electron microscopy and spectrum-imaging techniques were used to investigate the Co/Al2O3/graphene/SiO2 interfaces. Direct observation of pinhole contacts was achieved using FIB cross-sectional lamellas. Spatially resolved EDX spectrum profiles confirmed the presence of direct point contacts between the Co layer and the graphene. The high surface diffusion properties of graphene led to cluster-like Al2O3 film growth, limiting the minimal possible thickness for complete barrier coverage onto graphene surfaces using standard Al evaporation methods. The results indicate a minimum thickness of nominally 3 nm Al2O3, resulting in a 0.6 nm rms rough film with a maximum thickness reaching 5 nm.

Large size graphene (LSG) and multiwall carbon nanotubes (MWCNTs) on LSG were synthesized on a copper surface via chemical vapor deposition (CVD) at low temperature and normal pressure. The LSG were formed through an easy chemical cyclic reaction in which liquid benzene was heated to a temperature below its boiling point to create benzene vapors as graphene precursor material. The reaction mechanism was observed and the time-dependent analysis of the reaction revealed that mounds of the carbon nanotubes had grown as a result of the island that was found on the LSG sheet. The implications of the mechanism that we have introduced were investigated by coating a titanium sheet on the MWCNTs/LSG and LSG on the semiconductor electronic device. The photonic response was observed to be markedly high, which can be attributed to the positive synergetic effect between the Ti and LSG sheet of our prepared composites.

Large-area freestanding graphene films are facilely fabricated by reducing graphene oxide films on recyclable Cu foils in H2-containing atmosphere at high temperature. Cu might act as efficient catalysts for considerably improved reduction of graphene oxide according to the SEM, EDS, XRD, XPS, Raman and TGA results. Comparing to the graphene films with ~30 μm thickness reduced without Cu substrate at 900 °C, the thermal conductivity and electrical conductivity of graphene films reduced on Cu foils are enhanced about 140% to 902 Wm−1K−1 and 3.6 × 104 S/m, respectively. Moreover, the graphene films demonstrate superior thermal conductivity of ~1219 Wm−1K−1 as decreasing the thickness of films to ~10 μm. The graphene films also exhibit excellent mechanical properties and flexibility.

Oxic-settling-anaerobic process (OSA) was known as a cost-effective way to reduce the excess sludge production with simple upgrade of conventional activated sludge process (CAS). A low oxidation-reduction potential (ORP) level was the key factor to sludge decay and lysis in the sludge holding tank of the OSA process. However, the ORP control with nitrogen purge or chemical dosing in the OSA process would induce extra expense and complicate the operation. Hence, in this study, a sludge holding tank using gravity thickening was applied to OSA process to reduce the excess sludge production without any ORP control. Results showed that the modified OSA process not only reduced the excess sludge production effectively but also improved the sludge settleability without affected the treatment capacity. The reduction of the excess sludge production in the modified OSA process resulted from interactions among lots of factors. The key element of the process was the gravity thickening sludge holding tank.

In this work, a novel soft-hard template method towards the direct fabrication of graphene films on silicon/silica substrate is developed via a tri-constituent self-assembly route. Using cetyl trimethyl ammonium bromide (CTAB) as a soft template, silica (SiO2) from tetramethoxysilane as a hard template and pyrene as a carbon source, the self-assembly process allows the formation of a sandwich-like SiO2/CTAB/pyrene composite, which can be further converted to high quantity graphene films with a thickness of ~1 nm and a size of over 5 μm by thermal treatment. The morphology and thickness of the graphene films can be effectively controlled through the adjustment of the ratio of pyrene to CTAB. Furthermore, a high nonlinear refractive index n2 of ~10−12 m2 W−1 is measured from graphene/silica hybrid film, which is six orders of magnitude larger than that of silicon and comparable to the graphene from chemical vapor deposition process.

Graphene nucleation from crystalline Ni3C has been investigated using quantum chemical molecular dynamics (QM/MD) simulations based on the self-consistent-charge density-functional tight-binding (SCC-DFTB) method. It was observed that the lattice of Ni3C was quickly relaxed upon thermal annealing at high temperature, resulting in an amorphous Ni3C catalyst structure. With the aid of the mobile nickel atoms, inner layer carbon atoms precipitated rapidly out of the surface and then formed polyyne chains and Y-junctions. The frequent sinusoidal-like vibration of the branched carbon configurations led to the formation of nascent graphene precursors. In light of the rapid decomposition of the crystalline Ni3C, it is proposed that the crystalline Ni3C is unlikely to be a reaction intermediate in the CVD-growth of graphene at high temperatures. However, results present here indicate that Ni3C films can be employed as precursors in the synthesis of graphene with exciting possibility.