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• W2971831782 abstract "•N-Mo2C nanobelts with porous structure are uniformly synthesized•Nanocellulose is proposed to replace Nafion for binding powder catalysts•A facile strategy to prepare conductive film electrode is offered with practice•The flexible editable electrode exhibits excellent performance for scalable HER The large-scale application of economically efficient electrocatalysts for hydrogen evolution reaction (HER) is limited in view of the high cost of polymer binders (Nafion) for immobilizing of powder catalysts. In this work, nitrogen-doped molybdenum carbide nanobelts (N-Mo2C NBs) with porous structure are synthesized through a direct pyrolysis process using the pre-prepared molybdenum oxide nanobelts (MoO3 NBs). Nanocellulose instead of Nafion-bonded N-Mo2C NBs (N-Mo2[email protected]) exhibits superior performance toward HER, because of excellent dispersibility and multiple exposed catalytically active sites. Furthermore, the conductive film composed of N-Mo2C NBs, graphene nanosheets, and nanocellulose (N-Mo2C/[email protected]) is fabricated by simple vacuum filtration, as flexible and editable electrode, which possesses excellent performance for scale HER applications. This work not only proposes the potential of nanocellulose to replace Nafion for binding powder catalysts, but also offers a facile strategy to prepare flexible and conductive films for a wide variety of nanomaterials. The large-scale application of economically efficient electrocatalysts for hydrogen evolution reaction (HER) is limited in view of the high cost of polymer binders (Nafion) for immobilizing of powder catalysts. In this work, nitrogen-doped molybdenum carbide nanobelts (N-Mo2C NBs) with porous structure are synthesized through a direct pyrolysis process using the pre-prepared molybdenum oxide nanobelts (MoO3 NBs). Nanocellulose instead of Nafion-bonded N-Mo2C NBs (N-Mo2[email protected]) exhibits superior performance toward HER, because of excellent dispersibility and multiple exposed catalytically active sites. Furthermore, the conductive film composed of N-Mo2C NBs, graphene nanosheets, and nanocellulose (N-Mo2C/[email protected]) is fabricated by simple vacuum filtration, as flexible and editable electrode, which possesses excellent performance for scale HER applications. This work not only proposes the potential of nanocellulose to replace Nafion for binding powder catalysts, but also offers a facile strategy to prepare flexible and conductive films for a wide variety of nanomaterials. With the depletion of energy sources (such as oil and coal) and the environmental problems caused by burning fossil fuels (global warming, air and water pollution, etc.), green renewable energy sources such as solar energy and hydrogen energy are bound to become an important energy source for future development (Gray, 2009Gray H.B. Powering the planet with solar fuel.Nat. Chem. 2009; 1: 7Crossref PubMed Scopus (1362) Google Scholar, Turner, 2004Turner J.A. Sustainable hydrogen production.Science. 2004; 305: 972Crossref PubMed Scopus (4275) Google Scholar, Hui et al., 2019Hui L. Xue Y. Yu H. Liu Y. Fang Y. Xing C. Huang B. Li Y. Highly efficient and selective generation of ammonia and hydrogen on a graphdiyne-based catalyst.J. Am. Chem. Soc. 2019; https://doi.org/10.1021/jacs.9b03004Crossref Scopus (352) Google Scholar). Hydrogen energy is an extremely superior new energy source with high combustion heat value, no pollution, rich resources, and wide application range, which is regarded as the ideal clean energy in the future (Dresselhaus and Thomas, 2001Dresselhaus M.S. Thomas I.L. Alternative energy technologies.Nature. 2001; 414: 332Crossref PubMed Scopus (3611) Google Scholar, Yu et al., 2018aYu J. Li G. Liu H. Wang A. Yang L. Zhou W. Hu Y. Chu B. Simultaneous water recovery and hydrogen production by bifunctional electrocatalyst of nitrogen-doped carbon nanotubes protected cobalt nanoparticles.Int. J. Hydrogen Energy. 2018; 43: 12110-12118Crossref Scopus (12) Google Scholar, Yu et al., 2018bYu H. Xue Y. Hui L. Zhang C. Li Y. Zuo Z. Zhao Y. Li Z. Li Y. Efficient hydrogen production on a 3D flexible heterojunction material.Adv. Mater. 2018; 30: 1707082Crossref Scopus (135) Google Scholar). Among various hydrogen production procedures, electrochemical water splitting is inherently considered to be an ideal eco-friendly method to produce hydrogen with high purity (Koper, 2013Koper M.T.M. A basic solution.Nat. Chem. 2013; 5: 255Crossref PubMed Scopus (173) Google Scholar, Walter et al., 2010Walter M.G. Warren E.L. McKone J.R. Boettcher S.W. Mi Q. Santori E.A. Lewis N.S. Solar water splitting cells.Chem. Rev. 2010; 110: 6446-6473Crossref PubMed Scopus (7542) Google Scholar, Zeng et al., 2018Zeng L. Yang L. Lu J. Jia J. Yu J. Deng Y. Shao M. Zhou W. One-step synthesis of Fe-Ni hydroxide nanosheets derived from bimetallic foam for efficient electrocatalytic oxygen evolution and overall water splitting.Chin. Chem. Lett. 2018; 29: 1875-1878Crossref Scopus (63) Google Scholar, Yu et al., 2019Yu H. Xue Y. Huang B. Hui L. Zhang C. Fang Y. Liu Y. Zhao Y. Li Y. Liu H. Li Y. Ultrathin nanosheet of graphdiyne-supported palladium atom catalyst for efficient hydrogen production.iScience. 2019; 11: 31-41Abstract Full Text Full Text PDF PubMed Scopus (117) Google Scholar). Efficient water splitting typically requires highly active electrocatalysts to promote the hydrogen evolution reaction (HER) (Huang et al., 2018Huang Y. Ge J. Hu J. Zhang J. Hao J. Wei Y. Nitrogen-doped porous molybdenum carbide and phosphide hybrids on a carbon matrix as highly effective electrocatalysts for the hydrogen evolution reaction.Adv. Energy Mater. 2018; 8: 1701601Crossref Scopus (189) Google Scholar, Fang et al., 2019Fang Y. Xue Y. Hui L. Yu H. Liu Y. Xing C. Lu F. He F. Liu H. Li Y. In situ growth of graphdiyne based heterostructure: toward efficient overall water splitting.Nano Energy. 2019; 59: 591-597Crossref Scopus (63) Google Scholar). Recently, tremendous efforts have been devoted to search for non-precious metal catalysts to replace Platinum (Pt)-based catalysts in the hydrogen generation with high current densities at low overpotentials, which is thus highly desirable (Wang et al., 2016Wang J. Cui W. Liu Q. Xing Z. Asiri A.M. Sun X. Recent progress in cobalt-based heterogeneous catalysts for electrochemical water splitting.Adv. Mater. 2016; 28: 215-230Crossref PubMed Scopus (1828) Google Scholar, Shi and Zhang, 2016Shi Y. Zhang B. Recent advances in transition metal phosphide nanomaterials: synthesis and applications in hydrogen evolution reaction.Chem. Soc. Rev. 2016; 45: 1529-1541Crossref PubMed Google Scholar, Voiry et al., 2016Voiry D. Fullon R. Yang J. de Carvalho Castro e Silva C. Kappera R. Bozkurt I. Kaplan D. Lagos M.J. Batson P.E. Gupta G. et al.The role of electronic coupling between substrate and 2D MoS2 nanosheets in electrocatalytic production of hydrogen.Nat. Mater. 2016; 15: 1003Crossref PubMed Scopus (591) Google Scholar). In particular, as an alternative, molybdenum-based catalysts, such as molybdenum disulfide (MoS2) (Geng et al., 2016Geng X. Sun W. Wu W. Chen B. Al-Hilo A. Benamara M. Zhu H. Watanabe F. Cui J. Chen T.-P. Pure and stable metallic phase molybdenum disulfide nanosheets for hydrogen evolution reaction.Nat. Commun. 2016; 7: 10672Crossref PubMed Scopus (612) Google Scholar), molybdenum diselenide (MoSe2) (Deng et al., 2018Deng S. Yang F. Zhang Q. Zhong Y. Zeng Y. Lin S. Wang X. Lu X. Wang C.-Z. Gu L. et al.Phase modulation of (1T-2H)-MoSe2/TiC-C shell/core arrays via nitrogen doping for highly efficient hydrogen evolution reaction.Adv. Mater. 2018; 30: 1802223Crossref Scopus (198) Google Scholar), molybdenum phosphide (MoP) (Xiao et al., 2014Xiao P. Sk M.A. Thia L. Ge X. Lim R.J. Wang J.-Y. Lim K.H. Wang X. Molybdenum phosphide as an efficient electrocatalyst for the hydrogen evolution reaction.Energy Environ. Sci. 2014; 7: 2624-2629Crossref Google Scholar), molybdenum carbide (Mo2C) (Humagain et al., 2018Humagain G. MacDougal K. MacInnis J. Lowe J.M. Coridan R.H. MacQuarrie S. Dasog M. Highly efficient, biochar-derived molybdenum carbide hydrogen evolution electrocatalyst.Adv. Energy Mater. 2018; 8: 1801461Crossref Scopus (57) Google Scholar), and molybdenum nitride (MoN) (Zhang et al., 2016Zhang Y. Ouyang B. Xu J. Chen S. Rawat R.S. Fan H.J. 3D porous hierarchical nickel–molybdenum nitrides synthesized by RF plasma as highly active and stable hydrogen-evolution-reaction electrocatalysts.Adv. Energy Mater. 2016; 6: 1600221Crossref Scopus (426) Google Scholar), have recently attracted great attention as potential catalysts for HER, owing to their high cost-effectiveness, abundant molybdenum resources, favorable catalytic activities, and excellent stabilities (Xing et al., 2014Xing Z. Liu Q. Asiri A.M. Sun X. Closely interconnected network of molybdenum phosphide nanoparticles: a highly efficient electrocatalyst for generating hydrogen from water.Adv. Mater. 2014; 26: 5702-5707Crossref PubMed Scopus (730) Google Scholar, Vrubel and Hu, 2012Vrubel H. Hu X. Molybdenum boride and carbide catalyze hydrogen evolution in both acidic and basic solutions.Angew. Chem. Int. Ed. 2012; 124: 12875-12878Crossref Google Scholar, Xie et al., 2014Xie J. Zhang J. Li S. Grote F. Zhang X. Zhang H. Wang R. Lei Y. Pan B. Xie Y. Correction to controllable disorder engineering in oxygen-incorporated MoS2 ultrathin nanosheets for efficient hydrogen evolution.J. Am. Chem. Soc. 2014; 136: 1680Crossref Scopus (39) Google Scholar). Among them, Mo2C, an excellent transition metal carbide, has received increasing attention as a highly efficient HER electrocatalyst with high conductivity and optimal hydrogen absorption energy, in view of the fact that its electronic structure is almost identical to that of Pt-group elements (Wu et al., 2015Wu H.B. Xia B.Y. Yu L. Yu X.-Y. Lou X.W. Porous molybdenum carbide nano-octahedrons synthesized via confined carburization in metal-organic frameworks for efficient hydrogen production.Nat. Commun. 2015; 6: 6512Crossref PubMed Scopus (1139) Google Scholar, Zhao et al., 2015Zhao Y. Kamiya K. Hashimoto K. Nakanishi S. In situ CO2-emission assisted synthesis of molybdenum carbonitride nanomaterial as hydrogen evolution electrocatalyst.J. Am. Chem. Soc. 2015; 137: 110-113Crossref PubMed Scopus (252) Google Scholar, Wan et al., 2014Wan C. Regmi Y.N. Leonard B.M. Multiple phases of molybdenum carbide as electrocatalysts for the hydrogen evolution reaction.Angew. Chem. Int. Ed. 2014; 126: 6525-6528Crossref Google Scholar). To date, several kinds of Mo2C nanostructures have been successfully synthesized and showed the enhanced performance for HER (Wu et al., 2015Wu H.B. Xia B.Y. Yu L. Yu X.-Y. Lou X.W. Porous molybdenum carbide nano-octahedrons synthesized via confined carburization in metal-organic frameworks for efficient hydrogen production.Nat. Commun. 2015; 6: 6512Crossref PubMed Scopus (1139) Google Scholar, Yang et al., 2016Yang X. Feng X. Tan H. Zang H. Wang X. Wang Y. Wang E. Li Y. N-Doped graphene-coated molybdenum carbide nanoparticles as highly efficient electrocatalysts for the hydrogen evolution reaction.J. Mater. Chem. A. 2016; 4: 3947-3954Crossref Google Scholar, Xu et al., 2016Xu X. Nosheen F. Wang X. Ni-decorated molybdenum carbide hollow structure derived from carbon-coated metal–organic framework for electrocatalytic hydrogen evolution reaction.Chem. Mater. 2016; 28: 6313-6320Crossref Scopus (194) Google Scholar). It is well known that the electrocatalytic properties of metal carbides strongly depend on their surface structure and composition, which are closely associated with the porous structure and element doping (Wu et al., 2015Wu H.B. Xia B.Y. Yu L. Yu X.-Y. Lou X.W. Porous molybdenum carbide nano-octahedrons synthesized via confined carburization in metal-organic frameworks for efficient hydrogen production.Nat. Commun. 2015; 6: 6512Crossref PubMed Scopus (1139) Google Scholar, Wang et al., 2015Wang S. Wang J. Zhu M. Bao X. Xiao B. Su D. Li H. Wang Y. Molybdenum-carbide-modified nitrogen-doped carbon vesicle encapsulating nickel nanoparticles: a highly efficient, low-cost catalyst for hydrogen evolution reaction.J. Am. Chem. Soc. 2015; 137: 15753-15759Crossref PubMed Scopus (364) Google Scholar, Liu et al., 2015Liu Y. Yu G. Li G.-D. Sun Y. Asefa T. Chen W. Zou X. Coupling Mo2C with nitrogen-rich nanocarbon leads to efficient hydrogen-evolution electrocatalytic sites.Angew. Chem. Int. Ed. 2015; 127: 10902-10907Crossref Google Scholar). Huang et al. (Xiong et al., 2018Xiong J. Li J. Shi J. Zhang X. Suen N.-T. Liu Z. Huang Y. Xu G. Cai W. Lei X. et al.In situ engineering of double-phase interface in Mo/Mo2C heteronanosheets for boosted hydrogen evolution reaction.ACS Energy Lett. 2018; 3: 341-348Crossref Scopus (122) Google Scholar) prepared a kind of two-dimensional Mo/Mo2C heteronanosheets (Mo/Mo2C-HNS) as an efficient and stable noble metal-free electrocatalyst toward the HER in 0.5 M H2SO4. Gao et al. (Lin et al., 2016Lin H. Liu N. Shi Z. Guo Y. Tang Y. Gao Q. Cobalt-doping in molybdenum-carbide nanowires toward efficient electrocatalytic hydrogen evolution.Adv. Funct. Mater. 2016; 26: 5590-5598Crossref Scopus (353) Google Scholar) developed cobalt-doping into Mo2C nanowires to effectively optimize the electron features around Fermi level, accomplishing the efficient HER in both acidic and basic electrolytes. Therefore, to further improve HER activity of Mo2C, the structure-activity relationship relying on controlled morphology and doping for enhancing exposure of surface active sites is demanded to be uncovered for rational catalyst design. In addition, the agglomeration of catalysts, especially in the form of powder, can also lead to the loss of active sites (Chen et al., 2013Chen W.F. Wang C.H. Sasaki K. Marinkovic N. Xu W. Muckerman J.T. Zhu Y. Adzic R.R. Highly active and durable nanostructured molybdenum carbide electrocatalysts for hydrogen production.Energy Environ. Sci. 2013; 6: 943-951Crossref Scopus (789) Google Scholar). However, most of the as-synthesized nanoelectrocatalysts are in powder form, which need to be loaded onto glassy carbon (GC) electrodes with conductive polymer binders, such as Nafion. Unsatisfactorily, this step and the use of polymer materials will cause electrocatalysts agglomeration, which often leads to not only lower catalytic activity but also instability in the catalytic process (Asefa and Huang, 2017Asefa T. Huang X. Heteroatom-doped carbon materials for electrocatalysis.Chem. Eur. J. 2017; 23: 10703-10713Crossref PubMed Scopus (42) Google Scholar). Moreover, as long-term testing can cause Nafion to fall off from catalyst and electrode, resulting in poor contact between the catalyst particles and the underlying GC electrodes, the electron transfer from the electrode to electrocatalysts becomes difficult. Undoubtedly, Nafion is expensive and must undergo hazardous manufacturing processes, which is not suitable for large-scale practical applications (Liang et al., 2013Liang X. Zhang F. Feng W. Zou X. Zhao C. Na H. Liu C. Sun F. Zhu G. From metal–organic framework (MOF) to MOF–polymer composite membrane: enhancement of low-humidity proton conductivity.Chem. Sci. 2013; 4: 983-992Crossref Google Scholar, Dong et al., 2012Dong H. Yu H. Wang X. Zhou Q. Feng J. A novel structure of scalable air-cathode without Nafion and Pt by rolling activated carbon and PTFE as catalyst layer in microbial fuel cells.Water Res. 2012; 46: 5777-5787Crossref PubMed Scopus (378) Google Scholar, Kim et al., 2010Kim S. Yan J. Schwenzer B. Zhang J. Li L. Liu J. Yang Z. Hickner M.A. Cycling performance and efficiency of sulfonated poly (sulfone) membranes in vanadium redox flow batteries.Electrochem. Commun. 2010; 12: 1650-1653Crossref Scopus (217) Google Scholar). Therefore, it is urgently necessary to exploit a low-cost and readily available material that can bond the catalyst powder without reducing catalytic activity to replace the inconvenient artificial polymer, especially Nafion. Nanocelluloses (NCs), being an abundant and natural polymer with considerable physical and biological properties, including renewable resource, sustainability, excellent mechanical properties, biodegradability, and biocompatibility (Lin and Dufresne, 2014Lin N. Dufresne A. Nanocellulose in biomedicine: current status and future prospect.Eur. Polym. J. 2014; 59: 302-325Crossref Scopus (1082) Google Scholar, Geyer et al., 1994Geyer U. Heinze T. Stein A. Klemm D. Marsch S. Schumann D. Schmauder H.P. Formation, derivatization and applications of bacterial cellulose.Int. J. Biol. Macromol. 1994; 16: 343-347Crossref PubMed Scopus (88) Google Scholar), have been widely used in numerous fields such as electronics (Yan et al., 2014Yan C. Wang J. Kang W. Cui M. Wang X. Foo C.Y. Chee K.J. Lee P.S. Highly stretchable piezoresistive graphene–nanocellulose nanopaper for strain sensors.Adv. Mater. 2014; 26: 2022-2027Crossref PubMed Scopus (926) Google Scholar), medicine (Liu et al., 2007Liu Z. 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Moreover, nanocellulose possesses a superior hydrophilicity owing to the rich surface hydroxyl group, as well as high specific surface area and thermal stability, making it an advantageous carrier and binder for nanomaterials, especially in the powder form (Mo et al., 2009Mo Z.-l. Zhao Z.-l. Chen H. Niu G.-p. Shi H.-f. Heterogeneous preparation of cellulose–polyaniline conductive composites with cellulose activated by acids and its electrical properties.Carbohydr. Polym. 2009; 75: 660-664Crossref Scopus (121) Google Scholar, Kaushik and Moores, 2016Kaushik M. Moores A. Review: nanocelluloses as versatile supports for metal nanoparticles and their applications in catalysis.Green. Chem. 2016; 18: 622-637Crossref Google Scholar, Nyström et al., 2009Nyström G. Razaq A. Strømme M. Nyholm L. Mihranyan A. Ultrafast all-polymer paper-based batteries.Nano Lett. 2009; 9: 3635-3639Crossref PubMed Scopus (398) Google Scholar). In this work, we report nitrogen-doped molybdenum carbide nanobelts (N-Mo2C NBs) with porous structure synthesized through a direct pyrolysis process using the pre-prepared molybdenum oxide nanobelts (MoO3 NBs). Subsequently, nanocellulose instead of Nafion was employed in the bonding and fixing of N-Mo2C NBs. Surprisingly, nanocellulose bonded N-Mo2C NBs (N-Mo2[email protected]) exhibited superior performance for HER, which possessed a lower overpotential (achieved 10 mA cm−2) of 163 mV than Nafion bonded N-Mo2C NBs (N-Mo2[email protected]) (180 mV) in an acidic electrolyte. To develop a simple and inexpensive methodology for practical applications, the flexible film electrode composed of N-Mo2C NBs, graphene nanosheets, and nanocelluloses (N-Mo2C/[email protected]) was fabricated by vacuum filtration. The obtained N-Mo2C/[email protected] possessed a small onset potential of −41 mV versus RHE to reach 1 mA cm−2, low Tafel slope (58.83 mA dec−1), and superior long-term stability (remaining the current densities of 100 mA cm−2 for 100 h, 200 mA cm−2 for 77 h, and 300 mA cm−2 for 60 h with negligible degradation of 0.92%, 3.69%, and 4.04%, respectively) toward HER. This work not only proposed the potential of nanocellulose to replace Nafion for binding powder catalysts, but also offered a facile strategy to prepare flexible conductive film electrode for a wide variety of nanomaterials. Herein, we performed a detailed characterization of MoO3 NBs and N-Mo2C NBs. The MoO3 NBs with smooth surface were successfully synthesized by hydrothermal reaction, which was confirmed by scanning electron microscopy (SEM) image (Figure 1A), transmission electron microscopy (TEM) images (Figure S1), and X-ray powder diffraction (XRD, Figure S2). After calcining MoO3 NBs with dicyandiamide at 800°C for 2 h under Ar gas atmosphere, the prepared porous N-Mo2C NBs were confirmed by the XRD pattern (Figure 1H, JCPDS No. 72–1683), in which the characteristic peaks at 34.47° (021), 38.07° (200), 39.53° (121), 52.29° (221), 61.76° (040), 69.77° (321), 74.90° (240), and 75.85° (142) were detected (Wang et al., 2017Wang H. Sun C. Cao Y. Zhu J. Chen Y. Guo J. Zhao J. Sun Y. Zou G. Molybdenum carbide nanoparticles embedded in nitrogen-doped porous carbon nanofibers as a dual catalyst for hydrogen evolution and oxygen reduction reactions.Carbon. 2017; 114: 628-634Crossref Scopus (86) Google Scholar). Moreover, the SEM (Figures 1B and 1C) and TEM (Figures 1D and 1E) images indicated the nanobelt morphology of N-Mo2C with the width of ∼500 nm and length of 2–8 μm inherited from the pristine MoO3 NBs. However, the rough and porous surface of N-Mo2C NBs was observed. High-resolution transmission electron microscopy (HRTEM) image in Figure 1F revealed well-resolved lattice fringes with the interval distance of 0.223 nm that could be indexed to the (121) plane of Mo2C phase. The element mapping result exhibited a homogeneous distribution of the N, C, and Mo elements in the resultant N-Mo2C NBs (Figure 1G). Furthermore, the Brunauer-Emmett-Teller specific surface area of the porous N-Mo2C NBs was determined by N2 adsorption-desorption isotherm as 21.60 m2 g−1, which was larger than that of MoO3 NBs (11.03 m2 g−1), causing the penetration of electrolyte to be promoted and rich active sites to be exposed (Figure 1I) (Gao et al., 2016Gao X. Zhang H. Li Q. Yu X. Hong Z. Zhang X. Liang C. Lin Z. Hierarchical NiCo2O4 hollow microcuboids as bifunctional electrocatalysts for overall water-splitting.Angew. Chem. Int. Ed. 2016; 128: 6398-6402Crossref Google Scholar). Simultaneously, what we could get was that the pore size distribution of N-Mo2C was below 10 nm (inset of Figure 1I). Subsequently, the thicknesses of MoO3 NBs and N-Mo2C NBs were measured by atomic force microscope, as demonstrated in Figure S3. It could be observed that the thickness of the N-Mo2C NBs (∼120 nm) was greater than that of MoO3 NBs (∼58 nm), which should be derived from the rough porous structure formed on the surface of the N-Mo2C NBs, resulting in that N-Mo2C NBs possessed a larger specific surface area and exposed more catalytically active sites. Pleasantly, the N-Mo2C was steadily dispersed in nanocellulose aqueous solution, which maintained 24 h with negligible precipitation, as shown in Figure 2A. However, the N-Mo2C dispersed in both Nafion solution (Figure 2A) and aqueous solution (Figure S4) did not show satisfactory results. SEM was implemented to examine the morphologies and structures of N-Mo2[email protected] and N-Mo2[email protected] in Figures S5 and S6. As displayed in Figure S5, through the Nafion link, the N-Mo2C NBs were concentrated and buried, indicating that the use of Nafion would cause catalysts to aggregate and tightly cover catalysts, so that their active sites could not be fully exposed. On the contrary, in Figure S6, the morphology of the N-Mo2C NBs was maintained, and the addition of nanocelluloses caused the nanobelts to be bonded together and well fixed. Simultaneously, the N-Mo2C NBs could be fully released, which was beneficial to the exposure of active sites. To further confirm this point of view, the commercial 20 wt% Pt/C was taken the same dispersion in Nafion and nanocellulose solution. SEM in Figures S7 and S8 indicated that 20 wt% Pt/[email protected] possessed a higher exposure rate than that of 20 wt% Pt/[email protected] Next, we investigated the HER electrocatalytic activity of N-Mo2[email protected] modified GC electrode in an acidic electrolyte (0.5 M H2SO4), where the potential of the reference electrode was calibrated with respect to a reversible hydrogen electrode (RHE) performed in a high-purity H2 (99.999%)-saturated electrolyte (Figure S9). For comparison, the electrocatalytic actives of N-Mo2[email protected], 20 wt% Pt/[email protected], and 20 wt% Pt/[email protected] were also investigated as benchmarks under the same conditions, as displayed in Figure 2B. As expected, 20 wt% Pt/[email protected] behaved the best performance for HER among our catalysts, which only required an overpotential of 28 mV to reach a current density of 10 mA cm−2, which was lower than that of 20 wt% Pt/[email protected] catalyst (44 mV). Moreover, N-Mo2[email protected] possessed an overpotential (achieved 10 mA cm−2) of 163 mV lower than that of N-Mo2[email protected] catalyst (180 mV). When at a current density of 50 mA cm−2 or even higher, both 20 wt% Pt/[email protected] and N-Mo2[email protected] exhibited significant potential reductions of ∼38 mV compared with 20 wt% Pt/[email protected] and N-Mo2[email protected], respectively, indicating the potential of nanocellulose to replace Nafion for bonding powder catalysts. In addition, Tafel plots derived from Figure 2B indicated that the nanocellulose-bonded powder catalyst possessed a faster HER kinetics (Figure S10), further revealing the potential of nanocellulose to replace Nafion. The double-layer capacitance of N-Mo2[email protected] and N-Mo2[email protected] was measured by cyclic voltammograms (CVs), which was a pivotal parameter for estimating the electrochemical area at the solid-liquid interface. The double-layer capacitance of N-Mo2[email protected] (11.16 mF cm−2) was extremely larger than that of N-Mo2[email protected] (2.51 mF cm−2), as exhibited in Figures 2C and S11. The larger electrochemical area was associated with more active sites on the surface of N-Mo2[email protected] at the solid-liquid interface, which was driven from the double-layer capacitance. The HER kinetics of N-Mo2[email protected] and N-Mo2[email protected] at the electrode/electrolyte interface were further investigated in detail. In Figure 2D, the charge-transfer resistance (Rct) of N-Mo2[email protected] (31.8 Ω) was much lower than that of N-Mo2[email protected] (71.2 Ω), suggesting the favorable kinetics of N-Mo2[email protected] during the HER process. Figure 2E showed the representative Nyquist plots of N-Mo2[email protected] at various overpotentials. It could be seen that, as the overpotential increased, the diameter of the semicircle in the low frequency region decreased accordingly (60 Ω at 160 mV to 15 Ω at 280 mV), indicating a diminishment of Rct. In addition, to study the durability of N-Mo2[email protected], long-term stability tests at the constant potentials (250 and 320 mV) have been operated. As shown in Figure 2F, N-Mo2[email protected] displayed the current densities of 38 and 75 mA cm−2, which remained stable for 20 h with minimal degradation. Compared with N-Mo2[email protected], it could be observed from Figure S12 that N-Mo2[email protected] exhibited the obvious attenuation of 15.8% after i-t testing for 20 h. Therefore, the nanocellulose that replaced Nafion as binding agent was found to enhance not only the HER activity, but also the stability of the electrocatalyst. To reflect the practicality of film formation, loading on the surface of the substrate (carbon fiber cloth, abbreviated as CFC) was also achieved, which effectively reduced the amount of catalyst slurry. As manifested in Figures S13 and S14, N-Mo2[email protected] and 20 wt% Pt/[email protected] hybrid components were evenly distributed on the surface of carbon nanofibers. In addition, to highlight the performance advantages of nanocellulose in bonding powder catalysts compared with Nafion as a binder, additional five powder catalysts were further obtained, which were cobalt nanoparticles encapsulated in nitrogen-doped carbon nanotubes ([email protected]) obtained via an uncomplicated pyrolysis of Co-MOF (ZIF-67) (Yu et al., 2018aYu J. Li G. Liu H. Wang A. Yang L. Zhou W. Hu Y. Chu B. Simultaneous water recovery and hydrogen production by bifunctional electrocatalyst of nitrogen-doped carbon nanotubes protected cobalt nanoparticles.Int. J. Hydrogen Energy. 2018; 43: 12110-12118Crossref Scopus (12) Google Scholar, Yu et al., 2018bYu H. Xue Y. Hui L. Zhang C. Li Y. Zuo Z. Zhao Y. Li Z. Li Y. Efficient hydrogen production on a 3D flexible heterojunction material.Adv. Mater. 2018; 30: 1707082Crossref Scopus (135) Google Scholar), nitrogen-doped carbon nanotube-coated cobalt nanoparticles ([email protected]) by pyrolysis of cobalt salt with dicyandiamide, nitrogen-doped carbon nanotube-coated nickel nanoparticles ([email protected]) by pyrolysis of nickel salt with dicyandiamide (Zou et al., 2014Zou X. Huang X. Goswami A. Silva R. Sathe B.R. Mikmeková E. Asefa T. Cobalt-embedded nitrogen-rich carbon nanotubes efficiently catalyze hydrogen evolution reaction at all pH values.Angew. Chem. Int. Ed. 2014; 53: 4372-4376Crossref PubMed Scopus (841) Google Scholar, Zhou et al., 2016aZhou W. Lu J. Zhou K. Yang L. Ke Y. Tang Z. Chen S. CoSe2 nanoparticles embedded defective carbon nanotubes derived from MOFs as efficient electrocatalyst for hydrogen evolution reaction.Nano Energy. 2016; 28: 143-150Crossref Scopus (236) Google Scholar, Zhou et al., 2016bZhou W. Xiong T. Shi C. Zhou J. Zhou K. Zhu N. Li L. Tang Z. Chen S. Bioreduction of precious metals by microorganism: efficient [email protected] carbon electrocatalysts for the hydrogen evolution reaction.Angew." @default.
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• W2971831782 title "N-Doped Mo2C Nanobelts/Graphene Nanosheets Bonded with Hydroxy Nanocellulose as Flexible and Editable Electrode for Hydrogen Evolution Reaction" @default.
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