37 research outputs found
Selective Formation of C2 Products from Electrochemical CO<sub>2</sub> Reduction over Cu<sub>1.8</sub>Se Nanowires
Electrochemical
reduction of CO2 into higher-value C2 products (e.g., C2H4 and EtOH) is desirable for applications in chemical
and fuel industries. Herein, we report that Cu1.8Se nanowires
supported on Cu foam can function as an efficient electrocatalyst
for selective reduction of CO2 to C2 products, with the
Faradaic efficiencies for C2H4 and EtOH production
reaching 55% and 24% at −1.1 V, respectively. Additionally,
these nanowires also demonstrate a good long-term stability. We believe
that the high C2/C1 product selectivity exhibited by the resulting
catalyst is more likely due to a high CO2 pressure and
the presence of Se species
sj-docx-1-chl-10.1177_17475198211072812 – Supplemental material for A study on the preparation and performance of a graphene-supported, Ce ion-doped, high-efficiency, magnetic TiO2 photocatalyst
Supplemental material, sj-docx-1-chl-10.1177_17475198211072812 for A study on the preparation and performance of a graphene-supported, Ce ion-doped, high-efficiency, magnetic TiO2 photocatalyst by Weiyan Cao, Xijun Liu, Yuwei Wang, Yong Zhang and Congzhi Fu in Journal of Chemical Research</p
Ampere-Level Nitrate Electroreduction to Ammonia over Monodispersed Bi-Doped FeS<sub>2</sub>
Electrochemical conversion of NO3– into NH3 (NO3RR) holds an enormous prospect
to simultaneously yield valuable NH3 and alleviate NO3– pollution. Herein, we report monodispersed
Bi-doped FeS2 (Bi–FeS2) as a highly effective
NO3RR catalyst. Atomic coordination characterizations of
Bi–FeS2 disclose that the isolated Bi dopant coordinates
with its adjacent Fe atom to create the unconventional p–d
hybridized Bi–Fe dinuclear sites. Operando spectroscopic measurements
combined with theoretical calculations disclose that Bi–Fe
dinuclear sites can synergistically enhance the hydrogenation energetics
of NO3–-to-NH3 pathway, while
suppressing the competitive hydrogen evolution, leading to a high
NO3RR selectivity and activity. Consequently, the specially
designed flow cell equipped with Bi–FeS2 exhibits
a high NH3 yield rate of 83.7 mg h–1 cm–2 with a near-100% NO3–-to-NH3 Faradaic efficiency at an ampere-level current
density of 1023.2 mA cm–2, together with an excellent
long-term stability for 100 h of electrolysis, ranking almost the
highest performance among all reported NO3RR catalysts
High Selectivity Toward C<sub>2</sub>H<sub>4</sub> Production over Cu Particles Supported by Butterfly-Wing-Derived Carbon Frameworks
Converting
carbon dioxide to useful C2 chemicals in a selective
and efficient manner remains a major challenge in renewable and sustainable
energy research. Herein, we adopt butterfly wings to assist the preparation
of an electrocatalyst containing monodispersed Cu particles supported
by nitrogen-doped carbon frameworks for an efficient reduction of
CO<sub>2</sub>. Benefiting from structure advantages and the synergistic
effect between nitrogen dopants and stepped surface-rich Cu particles,
the resulting catalyst exhibited a high faradic efficiency of 63.7
± 1.4% for ethylene production (corresponding to an ethylene/methane
products’ ratio of 57.9 ± 5.4) and an excellent durability
(∼100% retention after 24 h). This work presents some guidelines
for the rational design and accurate modulation of metal heterocatalysts
for high selectivity toward ethylene from CO<sub>2</sub> electroreduction
Bifunctional BiPd Alloy Particles Anchored on Carbon Matrix for Reversible Zn–CO<sub>2</sub> Battery
Exploring reversible Zn–CO2 batteries holds great
promising potential for future CO2 fixation and energy
supply. Herein, the bifunctional PdBi alloy anchoring on carbon substrate
(BiPdC) is proposed for simultaneously catalyzing carbon dioxide reduction
reaction (CO2RR) and formic acid oxidation (FAO). The synergistic
effect between Pd and Bi overcomes the sluggish kinetics of CO2RR and FAO, causing the HCOOH Faraday efficiency (FEHCOOH) of 63.4% and 6.2 mA cm–2 current density for
FAO. Benefiting from the CO2–HCOOH interconversion,
the homemade reversible Zn–CO2 battery exhibits
the optimal 52.6% FEHCOOH and 1.1 V voltage gap within
45 h of cycling
Additional figures from Facile synthesis of Al-doped NiO nanosheet arrays for high-performance supercapacitors
XRD pattern, SEM image and galvanostatic discharge curve
Pd<sub>1</sub>Cu Single-Atom Alloys for High-Current-Density and Durable NO-to-NH<sub>3</sub> Electroreduction
Electrochemical
reduction of NO to NH3 (NORR)
offers
a prospective method for efficient NH3 electrosynthesis.
Herein, we first design single-atom Pd-alloyed Cu (Pd1Cu)
as an efficient and robust NORR catalyst at industrial-level current
densities (>0.2 A cm–2). Operando spectroscopic
characterizations and theoretical computations unveil that Pd1 strongly electronically couples its adjacent two Cu atoms
(Pd1Cu2) to enhance the NO activation while
promoting the NO-to-NH3 protonation energetics and suppressing
the competitive hydrogen evolution. Consequently, the flow cell assembled
with Pd1Cu exhibits an unprecedented NH3 yield
rate of 1341.3 μmol h–1 cm–2 and NH3–Faradaic efficiency of 85.5% at an industrial-level
current density of 210.3 mA cm–2, together with
an excellent long-term durability for 200 h of electrolysis, representing
one of the highest NORR performances on record
Hierarchical Zn<i><sub>x</sub></i>Co<sub>3–<i>x</i></sub>O<sub>4</sub> Nanoarrays with High Activity for Electrocatalytic Oxygen Evolution
The design and fabrication of efficient
and inexpensive electrodes
for use in the oxygen evolution reaction (OER) is essential for energy-conversion
technologies. In this study, high OER performance is achieved using
novel hierarchical Zn<sub><i>x</i></sub>Co<sub>3–<i>x</i></sub>O<sub>4</sub> nanostructures constructed with small
secondary nanoneedles grown on primary rhombus-shaped pillar arrays.
The nanostructures have large roughness factor, high porosity, and
high active-site density. Only a small overpotential of ∼0.32
V is needed for a current density of 10 mA/cm<sup>2</sup> with a Tafel
slope of 51 mV/decade. The nanostructures are also found to perform
significantly better than pure Co<sub>3</sub>O<sub>4</sub> and a commercial
Ir/C catalyst and to perform similarly to the best OER catalysts that
have been reported for alkaline media. These merits combined with
the satisfactory stability of the nanostructures indicate that they
are promising electrodes for water oxidation
Tremella-Like Ni–NiO with O‑Vacancy Heterostructure Nanosheets Grown In Situ on MXenes for Highly Efficient Hydrogen and Oxygen Evolution
Electronic modulation via heterostructures or vacancies
has been
recently regarded as an effective strategy to improve electrocatalytic
activity by optimizing the adsorption free energies of hydrogen evolution
reaction (HER) or oxygen evolution reaction (OER) active intermediates
during the reaction. Herein, tremella-like Ni–NiO with O-vacancy
heterostructure nanosheets grown in situ on Ti3C2Tx MXenes (Ni–NiO/Ti3C2Tx MXene) are fabricated
via a facile strategy. Benefitting from the heterointerfaces between
Ni and NiO, the synergetic coupling effects of MXenes and Ni–NiO
heterostructures, the O-vacancies, and the unique architecture, the
as-prepared Ni–NiO/Ti3C2Tx MXene showed superior activity toward the HER and
OER in alkaline electrolyte, only requiring overpotentials of 72 mV
for the HER and 248 mV for the OER to offer 10 mA cm–2. Density functional theory (DFT) calculations revealed that Ni–NiO
with O-vacancies can effectively increase the electron density around
the Fermi level and modulate the Gibbs free energies of the intermediates
during catalytic reactions, thus accelerating the reaction kinetics
Nanocellulose/Reduced Graphene Oxide Composite Hydrogels for High-Volumetric Performance Symmetric Supercapacitors
When graphene is used as an electrode material for supercapacitors,
it tends to have minor volumetric specific capacitance (<200 F
cm–3) and low volumetric energy density (<10
Wh L–1) due to its small packing density and poor
pseudocapacitive properties. Herein, nanocellulose/reduced graphene
oxide composite hydrogels (NCGHs) with a dense porous structure and
large packing density are prepared via a simple hydrothermal method
using graphene oxide (GO) and nanocellulose (NC) as a reacting substance.
In the reaction system, the high-concentration GO solution provides
the driving force for the formation of the dense porous structure
of NCGHs through the strong π–π stacking interaction
between graphene sheets. NC is used as a physical spacer, and its
main function is to inhibit the excessive aggregation of NCGHs. Moreover,
the super hydrophilicity of NC can also allow it to be used as an
electrolyte reservoir to promote the infiltration of NCGHs by the
electrolyte. Meanwhile, the oxygen-containing functional groups retained
in NCGHs after the hydrothermal reaction can also enhance their wettability
and pseudocapacitance. Consequently, the NCGH-40 based binder-less
symmetric supercapacitors delivers a high volumetric capacitance (351.8
F cm–3), a large volumetric energy density (12.2
Wh L–1), and a good rate capability of 80.4% even
at 10A g–1. Above all, a capacitance augment of
10.4% is achieved after 10,000 cycles at 10 A g–1, confirming its brilliant cycling stability. These parameters suggest
that NCGHs can be applied in next-generation energy storage devices
with high volumetric energy density
