Transient and general synthesis of high-density and ultrasmall nanoparticles on two-dimensional porous carbon via coordinated carbothermal shock DOI Creative Commons
Wenhui Shi, Zezhou Li, Zhihao Gong

и другие.

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Апрель 21, 2023

Abstract Carbon-supported nanoparticles are indispensable to enabling new energy technologies such as metal-air batteries and catalytic water splitting. However, achieving ultrasmall high-density (optimal catalysts) faces fundamental challenges of their strong tendency toward coarsening agglomeration. Herein, we report a general efficient synthesis uniformly dispersed on two-dimensional porous carbon. This is achieved through direct carbothermal shock pyrolysis metal-ligand precursors in just ~100 ms, the fastest among reported syntheses. Our results show that situ coordination (e.g., N → Co 2+ ) local ordering during millisecond-scale play crucial role kinetically dominated fabrication stabilization carbon films. The as-obtained samples exhibit excellent activity stability bifunctional catalysts oxygen redox reactions. Considering huge flexibility coordinated design, diversified single multielement (M = Fe, Co, Ni, Cu, Cr, Mn, Ag, etc) were generally fabricated, even systems well beyond traditional crystalline chemistry. method allows for transient well-dispersed with great simplicity versatility various application schemes.

Язык: Английский

Recent Progress on Rational Design of Bimetallic Pd Based Catalysts and Their Advanced Catalysis DOI
Jiaxuan Fan,

Haoxuan Du,

Zhao Yin

и другие.

ACS Catalysis, Год журнала: 2020, Номер 10(22), С. 13560 - 13583

Опубликована: Ноя. 10, 2020

Bimetallic Pd based catalysts have received tremendous research interests for many important reactions in fields of petrochemical industrial process, fine chemical synthesis, environment protection, renewable energy conversion, as their specific activity and selectivity are usually higher than that pure Pd. With a well-defined composition, Pd–M bimetallic also the ideal platform investigation reaction mechanism, which provides bridge construction high-performance catalyst. This Review intends to give an overview recent advances on design principles catalyst term active sites' structure number, provide insights into synergy effects between M well supports understand elementary mechanisms reactions. The starts with how intrinsic different structures (alloy, core–shell, Pd/metal compound interface) would be controlled by ligand effect, strain ensemble support effect; followed discussion determined mechanism selective hydrogenation, CO oxidation, methane combustion, electrocatalytic conversion (HER, ORR, MOR), CO2 reduction, H2 production, biomass upgrading, synthesis; then introduces strategies maximize number finite metal load. Finally, operando insight reconstruction under condition will discussed. On basis this Review, experience generic rules acquired from thoughts, synthetic disciplines, functionalities given could referential significance revealing catalytic at molecular scales building up other high-efficiency catalysts.

Язык: Английский

Процитировано

177

Multishell Hollow Metal/Nitrogen/Carbon Dodecahedrons with Precisely Controlled Architectures and Synergistically Enhanced Catalytic Properties DOI
Huirong Chen, Kui Shen,

Yongpeng Tan

и другие.

ACS Nano, Год журнала: 2019, Номер 13(7), С. 7800 - 7810

Опубликована: Июль 9, 2019

Multishell hollow nanoarchitectures are one of the most important branches in nanomaterial field due to their enormous potential many fields, but synthesizing them a well-controlled manner remains challenging. Herein, we present general strategy for construction multishell metal/nitrogen/carbon dodecahedrons (metal@NC) with well-defined and precisely controlled architectures. This is based on pyrolysis multilayer solid ZIFs prepared by step-by-step crystal growth approach, which enables precise control over shell number composition resultant metal@NC. Impressively, our can be further extended synthesis yolk@multishell structures or that assembled carbon nanotubes. The efficiently facilitate mass diffusion, together high dispersity increased surface area responsible significantly enhanced catalytic performances selective hydrogenation biomass-derived furfural cyclopentanol when compared single-shell counterparts. We anticipate would shed light rational design accurate other complex materials various yet challenging applications.

Язык: Английский

Процитировано

171

Scalable Synthesis of High Entropy Alloy Nanoparticles by Microwave Heating DOI
Haiyu Qiao,

Mahmoud Tamadoni Saray,

Xizheng Wang

и другие.

ACS Nano, Год журнала: 2021, Номер 15(9), С. 14928 - 14937

Опубликована: Авг. 23, 2021

High entropy alloy nanoparticles (HEA-NPs) are reported to have superior performance in catalysis, energy storage, and conversion due the broad range of elements that can be incorporated these materials, enabling tunable activity, excellent thermal chemical stability, a synergistic catalytic effect. However, scaling manufacturing HEA-NPs with uniform particle size homogeneous elemental distribution efficiently is still challenge required critical synthetic conditions where high temperature typically involved. In this work, we demonstrate an efficient scalable microwave heating method using carbon-based materials as substrates fabricate size. Due abundant functional group defects absorb efficiently, reduced graphene oxide employed model substrate produce average reaching ∼1850 K within seconds. As proof-of-concept, utilize rapid, high-temperature process synthesize PtPdFeCoNi HEA-NPs, which exhibit ∼12 nm mixing resulting from decomposition nearly at same time liquid metal solidification without diffusion. Various also substrates, including one-dimensional carbon nanofibers three-dimensional carbonized wood, achieve temperatures >1400 K. This facile compatible roll-to-roll process, providing feasible route for manufacturing.

Язык: Английский

Процитировано

171

Selective electrocatalytic semihydrogenation of acetylene impurities for the production of polymer-grade ethylene DOI
Jun Bu, Zhenpeng Liu, Wenxiu Ma

и другие.

Nature Catalysis, Год журнала: 2021, Номер 4(7), С. 557 - 564

Опубликована: Июль 1, 2021

Язык: Английский

Процитировано

156

High-performance ammonia oxidation catalysts for anion-exchange membrane direct ammonia fuel cells DOI
Yi Li, Hemanth Somarajan Pillai, Teng Wang

и другие.

Energy & Environmental Science, Год журнала: 2021, Номер 14(3), С. 1449 - 1460

Опубликована: Янв. 1, 2021

Low-temperature direct ammonia fuel cells (DAFCs) can use carbon-neutral as a fuel, which has attracted increasing attention recently due to ammonia's low source-to-tank energy cost, easy transport and storage, wide availability.

Язык: Английский

Процитировано

154

Ternary PtIrNi Catalysts for Efficient Electrochemical Ammonia Oxidation DOI
Yi Li, Xing Li, Hemanth Somarajan Pillai

и другие.

ACS Catalysis, Год журнала: 2020, Номер 10(7), С. 3945 - 3957

Опубликована: Март 3, 2020

Ammonia (NH3) has proved to be an effective alternative hydrogen in low-temperature fuel cells via its direct ammonia oxidation reaction (AOR). However, the kinetically sluggish AOR prohibitively hindered attractive cell (DAFC) applications. Here, we report efficient catalyst, which ternary PtIrNi alloy nanoparticles well dispersed on a binary composite support consisting of porous silicon dioxide (SiO2) and carboxyl-functionalized carbon nanotube (PtIrNi/SiO2-CNT-COOH) through sonochemical-assisted synthesis method. The nanoparticles, with aid abundant OHad provided by SiO2 improved electrical conductivity CNTs, exhibit remarkable catalytic activity for alkaline media. It is evidenced lower onset potential (∼0.40 V vs reversible electrode (RHE)) at room temperature than that commercial PtIr/C (ca. 0.43 RHE). Increasing NH3 concentrations operation temperatures can significantly enhance this nanoparticle catalyst. Specifically, catalyst 80 °C exhibits much (∼0.32 RHE) higher peak current density, indicating DAFCs operated are favorable increased performance. Constant-potential density functional theory (DFT) calculations showed Pt–Ir ensembles {100}-terminated surfaces serve as active site. introduction Ni raises center energy states projected onto group d-orbitals surface sites thus lowers theoretical *NH2 dehydrogenation *NH compared Pt Pt3Ir alloy.

Язык: Английский

Процитировано

153

Confining ultrasmall bimetallic alloys in porous N–carbon for use as scalable and sustainable electrocatalysts for rechargeable Zn–air batteries DOI
Jingjing Liu, Ting He, Qichen Wang

и другие.

Journal of Materials Chemistry A, Год журнала: 2019, Номер 7(20), С. 12451 - 12456

Опубликована: Янв. 1, 2019

Ultrasmall bimetallic alloy nanoparticles are generated via a micro–mesopore confinement synthesis strategy in nanoporous N–carbon. The prepared catalysts show excellent bifunctional performance both ORR and OER, outstanding energy conversion efficiency Zn–air batteries.

Язык: Английский

Процитировано

151

A General Strategy to Atomically Dispersed Precious Metal Catalysts for Unravelling Their Catalytic Trends for Oxygen Reduction Reaction DOI
Jae Hyung Kim,

Dongyup Shin,

Jaekyoung Lee

и другие.

ACS Nano, Год журнала: 2020, Номер 14(2), С. 1990 - 2001

Опубликована: Янв. 30, 2020

Atomically dispersed precious metal catalysts have emerged as a frontier in catalysis. However, robust, generic synthetic strategy toward atomically is still lacking, which has limited systematic studies revealing their general catalytic trends distinct from those of conventional nanoparticle (NP)-based catalysts. Herein, we report catalysts, consists "trapping" precursors on heteroatom-doped carbonaceous layer coated carbon support and "immobilizing" them with SiO2 during thermal activation. Through the "trapping-and-immobilizing" method, five (Os, Ru, Rh, Ir, Pt) could be obtained served model for unravelling oxygen reduction reaction (ORR). Owing to isolated geometry, generally showed higher selectivity H2O2 production than NP counterparts ORR. Among was changed by types metals, Pt catalyst showing highest selectivity. A combination experimental results density functional theory calculations revealed that trend correlated binding energy difference between *OOH *O species. In terms 2 e- ORR activity, Rh best activity. Our approach may help understanding unique behaviors

Язык: Английский

Процитировано

148

Preparation of the Catalysts DOI
Shuiping Luo, Min Tang,

Yujia Liao

и другие.

Springer eBooks, Год журнала: 2021, Номер unknown, С. 183 - 214

Опубликована: Янв. 1, 2021

Язык: Английский

Процитировано

137

Recent advances in ruthenium(II) and iridium(III) complexes containing nanosystems for cancer treatment and bioimaging DOI
Jinchao Shen, Thomas W. Rees,

Liang‐Nian Ji

и другие.

Coordination Chemistry Reviews, Год журнала: 2021, Номер 443, С. 214016 - 214016

Опубликована: Май 20, 2021

Язык: Английский

Процитировано

104