Jiangbo Xi

Freestanding Graphene Paper Supported Three-Dimensional Porous Graphene–Polyaniline Nanocomposite Synthesized by Inkjet Printing and in Flexible All-Solid-State Supercapacitor

Freestanding paper-like electrode materials have trigged significant research interest for their practical application in flexible and lightweight energy storage devices. In this work, we reported a new type of flexible nanohybrid paper electrode based on full inkjet printing synthesis of a freestanding graphene paper (GP) supported three-dimensional (3D) porous graphene hydrogel (GH)-polyaniline (PANI) nanocomposite, and explored its practical application in flexible all-solid-state supercapacitor (SC). The utilization of 3D porous GH scaffold to load nanostructured PANI dramatically enhances the electrical conductivity, the specific capacitance and the cycle stability of the GH-PANI nanocomposite. Additionally, GP can intimately interact with GH-PANI through π-π stacking to form a unique freestanding GP supported GH-PANI nanocomposite (GH-PANI/GP) with distinguishing mechanical, electrochemical and capacitive properties. These exceptional attributes, coupled with the merits of full inkjet printing strategy, lead to the formation of a high-performance binder-free paper electrode for flexible and lightweight SC application. The flexible all-solid-state symmetric SC based on GH-PANI/GP electrode and gel electrolyte exhibits remarkable mechanical flexibility, high cycling performance and acceptable energy density of 24.02 Wh kg(-1) at a power density of 400.33 W kg(-1). More importantly, the proposed simple and scale-up full inkjet printing procedure for the preparation of freestanding GP supported 3D porous GH-PANI nanocomposite is a modular approach to fabricate other graphene-based nanohybrid papers with tailorable properties and optimal components.

Encapsulating Pd nanoparticles in double-shelled graphene@carbon hollow spheres for excellent chemical catalytic property.

Double-shelled hollow carbon spheres with reduced graphene oxide (RGO) as inner shell and carbon (C) layer as outer shell have been successfully designed and prepared. This tailor-making structure acts as an excellent capsule for encapsulating with ultrafine Pd nanoparticles (Pd NPs), which could effectively prevent Pd NPs from aggregation and leaching. As a result, the as-obtained RGO@Pd@C nanohybid exhibits superior and stable catalytic performance. With the aid of RGO@Pd@C, the reduction reaction of 4-nitrophenol (4-NP) to 4-aminophenol with NaBH4 as reducing agent can be finished within only 30 s, even the content of Pd is as low as 0.28 wt%. As far as we know, RGO@Pd@C is one of the most effective catalyst for 4-NP reducing reaction up to now.

Ultrafine Pd Nanoparticles Encapsulated in Microporous Co3O4 Hollow Nanospheres for In Situ Molecular Detection of Living Cells

Recent progress in the in situ molecular detection of living cells has attracted tremendous research interests due to its great significance in biochemical, physiological, and pathological investigation. Especially for the electrochemical detection of hydrogen peroxide (H2O2) released by living cells, the highly efficient and cost-effective electrocatalysts are highly desirable. In this work, we develop a novel type of microporous Co3O4 hollow nanospheres containing encapsulated Pd nanoparticles (Pd@Co3O4). Owing to the synergy effect between the permeable microporous Co3O4 shell and the ultrafine Pd nanoparticles that encapsulated in it, the resultant Pd@Co3O4 based electrode exhibits excellent electrochemical sensor performance toward H2O2, even when the content of Pd in Pd@Co3O4 hollow nanospheres is as low as 1.14 wt %, which enable it be used for real-time tracking of the secretion of H2O2 in different types of living human cells.

Mussel-inspired Functionalization of Cotton for Nano-catalyst Support and Its Application in a Fixed-bed System with High Performance

Inspired by the composition of adhesive and reductive proteins secreted by marine mussels, polydopamine (PDA) was used to coat cotton microfiber (CMF), and then acted as reducing agent for the growth of Pd nanoparticles on PDA coated CMF (PDA@CMF) composites. The resultant CMF@PDA/Pd composites were then packed in a column for the further use in fixed-bed system. For the catalysis of the reduction of 4-nitrophenol, the flow rate of the 4-aminophenol solution (0.5 mM) was as high as 60 mL/min. The obtained fixed-bed system even exhibited superior performance to conventional batch reaction process because it greatly facilitated the efficiency of the catalytic fibers. Consequently, its turnover frequency (TOF) was up to 1.587 min−1, while the TOF in the conventional batch reaction was 0.643 min−1. The catalytic fibers also showed good recyclability, which can be recycled for nine successive cycles without a loss of activity. Furthermore, the catalytic system based on CMF@PDA/Pd can also be applied for Suzuki coupling reaction with the iodobenzene conversion up to 96.7%. The strategy to prepare CMF@PDA/Pd catalytic fixed bed was simple, economical and scalable, which can also be applied for coating different microfibers and loading other noble metal nanoparticles, was amenable for automated industrial processes.

Raisin bread-like iron sulfides/nitrogen and sulfur dual-doped mesoporous graphitic carbon spheres: a promising electrocatalyst for the oxygen reduction reaction in alkaline and acidic media

A raisin bread-like electrocatalyst composed of iron sulfides (Fe1−xS) and nitrogen and sulfur dual-doped mesoporous graphitic carbon spheres (N, S-MGCSs) is successfully synthesized via a two-step pyrolysis and acid leaching process. The resulting Fe1−xS/N, S-MGCS catalysts demonstrate excellent electrocatalytic activities towards the oxygen reduction reaction (ORR) in alkaline and acidic media, the activities of which are closely related to the content and distribution of iron sulfide species. The most optimized electrocatalytic activity achieved over (Fe1−xS/N, S-MGCS)0.2 even outperforms that of the commercial Pt/C catalyst in alkaline media, and is close to that of highly active non-precious metal catalysts reported so far in acidic media. The remarkable catalytic performance is ascribed to the iron sulfide nanocrystals introduced into the highly conductive carbon supports for significantly enhancing the reactivity of catalytically active sites, and the raisin bread-like structure constructed for improving the characteristics of electron and ion transport and inhibiting the self-aggregation and leaching of iron sulfide species. Moreover, this work inspires a new consideration in the field for understanding the catalytic roles of the doped carbon species and transition metal chalcogenides during the ORR electrocatalysis.

Coordination-Assisted Polymerization of Mesoporous Cobalt Sulfide/Heteroatom (N,S)-Doped Double-Layered Carbon Tubes as an Efficient Bifunctional Oxygen Electrocatalyst

It is a critical challenge to construct efficient precious-metal-free bifunctional oxygen electrocatalysts for fuel cell and metal-air batteries via structural and component engineering. Herein, a one-dimensional mesoporous double-layered tubular structure, where Co9S8 nanocrystals are incorporated into nitrogen, sulfur codoped carbon, is successfully synthesized via the coordinated-assisted polymerization and sacrificial template methods. The double-layered tubular structure provides for a large electrochemically active surface area and promotes fast mass transfer. Cobalt oxides/oxyhydroxides, which are evolved from the sulfides during the catalytic processes, as the main active sites efficiently catalyze the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), in cooperation with the Co-N-C and heteroatom-induced active sites. Hence, it demonstrates excellent bifunctional electrocatalytic activity with the overvoltage between the OER potential at 10 mA cm-2 ( E10) and ORR half-wave potential ( E1/2) of 0.707 V, which is superior to most of precious-metal-free bifunctional oxygen electrocatalysts reported recently, as well as the state-of-art Pt/C and RuO2 catalysts.