Yi Shi

Activated carbon with ultrahigh specific surface area synthesized from natural plant material for lithium–sulfur batteries

Porous activated carbon with a ultrahigh specific surface area (3164 m2 g−1) and large pore volume (1.88 cm3 g−1) was prepared from waste litchi shells with channel-like macropores via a KOH activation method. The macroporous structure of litchi shells is believed to be conducive to distribute the activation agent, which enables sufficient activation. The as-prepared activated carbon was developed as a conducting framework for lithium–sulfur battery cathode materials. The resulting activated carbon/sulfur composite cathode possesses a high specific capacity, good rate capability, and long-term cycling performance. At 200 mA g−1 current density, the initial discharge capacity of the activated carbon/sulfur composite cathode with 60 wt% sulfur content is 1105 mA h g−1. At a current density of 800 mA g−1, the activated carbon/sulfur composite cathode shows 51% capacity retention over 800 cycles with a fade rate of 0.06% per cycle. The coulombic efficiency of the cell remains at approximately 95%. By adding LiNO3 in the electrolyte, the activated carbon/sulfur composite electrode tested at 800 mA g−1 shows a high coulombic efficiency (>99%). The activated carbon/sulfur composites exhibited similar capacity value and cycling trends with an increase in sulfur content from 60% to 68%. The good electrochemical performance can be attributed to the excellent structural parameters of the activated carbon. The ultrahigh specific surface area and large pore volume not only enhances the sulfur content but also ensures dispersion of elemental sulfur in the conducting framework, thereby improving sulfur utilization. The small nanopores of the activated carbon can effectively inhibit the diffusion of polysulfides during the charge/discharge process.

Hollow Core–Shell Structured Ni–Sn@C Nanoparticles: A Novel Electrocatalyst for the Hydrogen Evolution Reaction

Pt-free electrocatalysts with high activity and low cost are highly pursued for hydrogen production by electrochemically splitting water. Ni-based alloy catalysts are potential candidates for the hydrogen evolution reaction (HER) and have been studied extensively. Here, we synthesized novel hollow core-shell structure Ni-Sn@C nanoparticles (NPs) by sol-gel, chemical vapor deposition, and etching processes. The prepared electrocatalysts with porous hollow carbon layers have a high conductivity and large active area, which exhibit good electrocatalytic activity toward HER. The Tafel slope of ∼35 millivolts per decade measured in acidic solution for Ni-Sn@C NPs is the smallest one to date for the Ni-Sn alloy catalysts, and exceeds those of the most non-noble metal catalysts, indicating a possible Volmer-Heyrovsky reaction mechanism. The synthetic method can be extended to prepare other hollow core-shell structure electrocatalysts for low-temperature fuel cells.

Direct Plasmon-Accelerated Electrochemical Reaction on Gold Nanoparticles

Direct photocatalysis making use of plasmonic metals has attracted significant attention due to the light-harnessing capabilities of these materials associated with localized surface plasmon resonance (LSPR) features. Thus far, most reported work has been limited to plasmon-induced chemical transformations. Herein, we demonstrate that electrochemical reactions can also be accelerated by plasmonic nanoparticles upon LSPR excitation. Using glucose electrocatalysis as a model reaction system, the direct plasmon-accelerated electrochemical reaction (PAER) on gold nanoparticles is observed. The wavelength- and solution-pH-dependent electrochemical oxidation rate and the dark-field scattering spectroscopy results confirm that the hot charge carriers generated during plasmon decay are responsible for the enhanced electrocatalysis performance. Based on the proposed PAER mechanism, a plasmon-improved glucose electrochemical sensor is constructed, demonstrating the enhanced performance of the non-enzyme sensor upon LSPR excitation. This plasmon-accelerated electrochemistry promises potential applications in (bio)electrochemical energy conversion, electroanalysis, and electrochemical devices.

Enhanced Peroxidase‐Like Performance of Gold Nanoparticles by Hot Electrons

Enzyme mimics have been widely used as alternatives to natural enzymes. However, the catalytic performances of enzyme mimics are often decreased due to different spatial structures or absence of functional groups compared to natural enzymes. Here, we report a highly efficient enzyme-like catalytic performance of gold nanoparticles (AuNPs) by visible-light stimulation. The enzyme-like reaction is evaluated by the catalytic reaction of AuNPs oxidizing a typical chromogenic substrate 3,3,5,5-tetramethylbenzydine (TMB) with hydrogen peroxide as an oxidant. From investigations of the wavelength-dependent reaction rate, radical capture, hole-donor addition, and dark-field scattering spectroscopy experiments, it is revealed that the strong plasmonic absorption of AuNPs facilitates generation of hot electrons, which are transfered from AuNPs to the adsorbed reactant molecule, greatly promoting the catalytic performance of the enzyme-like catalytic reaction. The present work provides a simple method for improving the performance of enzyme mimics, which is expected to find further application in the field of plasmon-enhanced biocatalysis and biosensors.

Generalized Low-Temperature Fabrication of Scalable Multi-Type Two-Dimensional Nanosheets with a Green Soft Template

Two-dimensional nanosheets with high specific surface areas and fascinating physical and chemical properties have attracted tremendous interests because of their promising potentials in both fundamental research and practical applications. However, the problem of developing a universal strategy with a facile and cost-effective synthesis process for multi-type ultrathin 2 D nanostructures remains unresolved. Herein, we report a generalized low-temperature fabrication of scalable multi-type 2 D nanosheets including metal hydroxides (such as Ni(OH)2, Co(OH)2, Cd(OH)2, and Mg(OH)2), metal oxides (such as ZnO and Mn3O4), and layered mixed transition-metal hydroxides (Ni-Co LDH, Ni-Fe LDH, Co-Fe LDH, and Ni-Co-Fe layered ternary hydroxides) through the rational employment of a green soft-template. The synthesized crystalline inorganic nanosheets possess confined thickness, resulting in ultrahigh surface atom ratios and chemically reactive facets. Upon evaluation as electrode materials for pseudocapacitors, the Ni-Co LDH nanosheets exhibit a high specific capacitance of 1087 F g(-1) at a current density of 1 A g(-1), and excellent stability, with 103% retention after 500 cycles. This strategy is facile and scalable for the production of high-quality ultrathin crystalline inorganic nanosheets, with the possibility of extension to the preparation of other complex nanosheets.

A simple way to fine tune the redox potentials of cobalt ions encapsulated in nitrogen doped graphene molecular catalysts for the oxygen evolution reaction

Co2+ ions encapsulated in nitrogen doped graphene were applied as an oxygen evolution catalyst. Their redox potentials were tuned using different counter anions as liable ligands, and the redox potential related catalytic rates were explored. It was proposed that the electron density of Co2+ ions was a general descriptor for activity.