Highly Efficient Transformation of Tar Model Compounds into Hydrogen by a Ni–Co Alloy Nanocatalyst During Tar Steam Reforming DOI
Junjie Chen,

Yongxiao Liu,

Zhengrui Chen

et al.

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: unknown

Published: Feb. 6, 2024

Hydrogen (H2) production from coal and biomass gasification was considered a long-term viable way to solve energy crises global warming. Tar, generated as hazardous byproduct, limited its large-scale applications by clogging corroding equipment. Although catalytic steam reforming technology used convert tar into H2, catalyst deactivation restricted applicability. A novel nanocatalyst first synthesized the modified sol–gel method using activated biochar support, nickel (Ni) active component, cobalt (Co) promoter for converting H2. The results indicated that high H2 yield of 263.84 g H2/kg TMCs (Tar Model Compounds) TMC conversion almost 100% were obtained over 6% Ni–4% Co/char, with more than 30% increase in hydrogen compared traditional catalysts. Moreover, Co/char exhibited excellent resistance carbon deposition removing nucleation sites graphite formation, forming stable Ni–Co alloy, promoting char reaction; oxidation due oxygen affinity Co reduction oxidized CO; sintering strengthened interaction between Ni Co, specific surface area (920.61 m2/g), dispersion (7.3%) nanoparticles. This work provided significant potential practical situ during reforming.

Language: Английский

High-entropy alloys in electrocatalysis: from fundamentals to applications DOI
Jin‐Tao Ren, Lei Chen, Haoyu Wang

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(23), P. 8319 - 8373

Published: Jan. 1, 2023

In this review, we provide a comprehensive summary of recent advances in the synthesis strategies, design principles, and characterization technologies high entropy alloys, their applications various electrocatalytic conversion reactions.

Language: Английский

Citations

169
Unveiling the Reaction Mechanism of Nitrate Reduction to Ammonia Over Cobalt-Based Electrocatalysts DOI

Kaiwen Yang,

Shuhe Han, Chuanqi Cheng

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(19), P. 12976 - 12983

Published: April 3, 2024

Electrocatalytic reduction of nitrate to ammonia (NRA) has emerged as an alternative strategy for sewage treatment and generation. Despite excellent performances having been achieved over cobalt-based electrocatalysts, the reaction mechanism well veritable active species across a wide potential range are still full controversy. Here, we adopt CoP, Co, Co3O4 model materials solve these issues. CoP evolves into core@shell structured CoP@Co before NRA. For Co catalysts, three-step relay is carried out superficial dynamical Coδ+ under low overpotential, while continuous hydrogenation from unveiled high overpotential. In comparison, stable steadily catalyze range. As result, exhibit much higher NRA activity than especially Moreover, performance although they experience same mechanism. A series characterizations clarify reason enhancement highlighting that core donates abundant electrons species, leading generation more hydrogen nitrogen-containing intermediates.

Language: Английский

Citations

79
Ultrathin Rh Nanosheets with Rich Grain Boundaries for Efficient Hydrogen Oxidation Electrocatalysis DOI
Xiaodong Yang, Bo Ouyang, Lei Zhao

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(49), P. 27010 - 27021

Published: Nov. 10, 2023

Two-dimensional (2D) Pt-group ultrathin nanosheets (NSs) are promising advanced electrocatalysts for energy-related catalytic reactions. However, improving the electrocatalytic activity of 2D NSs through addition abundant grain boundaries (GBs) and understanding underlying formation mechanism remain significant challenges. Herein, we report controllable synthesis a series Rh-based nanocrystals (e.g., Rh nanoparticles, NSs, with GBs) CO-mediated kinetic control route. In light NSs' structural advantages GB modification, rich GBs exhibit an enhanced compared to pure commercial Pt/C toward hydrogen oxidation reaction (HOR) in alkaline media. Both experimental results theoretical computations corroborate that have capacity ameliorate adsorption free energy intermediates during HOR, thus resulting outstanding HOR performance. Our work offers novel perspectives realm developing sophisticated metal conversion field.

Language: Английский

Citations

59
Unveiling synergy of strain and ligand effects in metallic aerogel for electrocatalytic polyethylene terephthalate upcycling DOI
J.T. Chen, Fangzhou Zhang,

Min Kuang

et al.

Proceedings of the National Academy of Sciences, Journal Year: 2024, Volume and Issue: 121(17)

Published: April 17, 2024

Recently, there has been a notable surge in interest regarding reclaiming valuable chemicals from waste plastics. However, the energy-intensive conventional thermal catalysis does not align with concept of sustainable development. Herein, we report electrocatalytic approach allowing selective synthesis glycolic acid (GA) polyethylene terephthalate (PET) over Pd 67 Ag 33 alloy catalyst under ambient conditions. Notably, delivers high mass activity 9.7 A mg −1 for ethylene glycol oxidation reaction (EGOR) and GA Faradaic efficiency 92.7 %, representing most active synthesis. In situ experiments computational simulations uncover that ligand effect induced by incorporation enhances selectivity facilitating carbonyl intermediates desorption, while lattice mismatch-triggered tensile strain optimizes adsorption *OH species to boost kinetics. This work unveils synergistic provides guidance design future catalysts PET upcycling. We further investigate versatility on CO 2 reduction (CO RR) assemble EGOR//CO RR integrated electrolyzer, presenting pioneering demonstration reforming carbon resource (i.e., ) into high-value chemicals.

Language: Английский

Citations

35
Bimetallic nanoalloys planted on super-hydrophilic carbon nanocages featuring tip-intensified hydrogen evolution electrocatalysis DOI Creative Commons
Linjie Zhang, Haihui Hu,

Chen Sun

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Aug. 21, 2024

The insufficient availability and activity of interfacial water remain a major challenge for alkaline hydrogen evolution reaction (HER). Here, we propose an "on-site disruption near-site compensation" strategy to reform the bonding network via deliberate cation penetration catalyst support engineering. This concept is validated using tip-like bimetallic RuNi nanoalloys planted on super-hydrophilic high-curvature carbon nanocages (RuNi/NC). Theoretical simulations suggest that tip-induced localized concentration hydrated K+ facilitates optimization dynamics intermediate adsorption. In situ synchrotron X-ray spectroscopy endorses H* spillover-bridged Volmer‒Tafel mechanism synergistically relayed between Ru Ni. Consequently, RuNi/NC exhibits low overpotential 12 mV high durability 1600 h at 10 mA cm‒2 HER, demonstrates performance in both electrolysis chlor-alkali electrolysis. offers microscopic perspective design manipulation local structure toward enhanced HER kinetics. A with optimized H2 reported. designed shows catalytic by achieving 13.6-fold higher mass than Pt/C.

Language: Английский

Citations

29
Ordered Mesoporous Crystalline Frameworks Toward Promising Energy Applications DOI
Jialong Li,

Rongyao Li,

Wendi Wang

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(16)

Published: Jan. 2, 2024

Abstract Ordered mesoporous crystalline frameworks (MCFs), which possess both functional and well‐defined porosity, receive considerable attention because of their unique properties including high surface areas, large pore sizes, tailored porous structures, compositions. Construction novel architectures that allows for rich accessible active sites efficient mass transfer is envisaged to offer ample opportunities potential energy‐related applications. In this review, the rational synthesis, energy applications MCFs are main focus. After summarizing synthetic approaches, an emphasis placed on delicate control crystallites, mesophases, nano‐architectures by concluding basic principles showing representative examples. Afterward, currently fabricated components such as metals, metal oxides, sulfides, metal–organic described in sequence. Further, typical rechargeable batteries, supercapacitors, electrocatalysis, photocatalysis highlighted. This review ends with possible development challenges well a future prospect high‐efficiency applications, underscores pathway developing advanced materials.

Language: Английский

Citations

26
FeCoCuMnRuB Nanobox with Dual Driving of High-Entropy and Electron-Trap Effects as the Efficient Electrocatalyst for Water Oxidation DOI
Li Liu, Tinghui Liu,

Can Xu

et al.

Nano Letters, Journal Year: 2024, Volume and Issue: 24(9), P. 2831 - 2838

Published: Feb. 22, 2024

High-entropy borides hold potential as electrocatalysts for water oxidation. However, the synthesis of tailored nanostructures remains a challenge due to thermodynamic immiscibility polymetallic components. Herein, FeCoCuMnRuB nanobox decorated with nanosheet array was synthesized first time by "coordination-etch-reduction" method. The has various structural characteristics express catalytic performance; meanwhile, it combines high-entropy effect multiple components electron trap induced electron-deficient B, synergistically regulating its electronic structure. As result, exhibits enhanced OER activity low overpotential (η10 = 233 mV), high TOF value (0.0539 s–1), small Tafel slope (61 mV/dec), and satisfactory stability 200 h, outperforming alloy low-entropy borides. This work develops entropy B-driven strategy motivating performance oxidation, which broadens diversity category materials.

Language: Английский

Citations

22
Isolated Octahedral Pt-Induced Electron Transfer to Ultralow-Content Ruthenium-Doped Spinel Co3O4 for Enhanced Acidic Overall Water Splitting DOI
Di Li,

Danyun Xu,

Yuhou Pei

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 13, 2024

The development of a highly active and stable oxygen evolution reaction (OER) electrocatalyst is desirable for sustainable efficient hydrogen production via proton exchange membrane water electrolysis (PEMWE) powered by renewable electricity yet challenging. Herein, we report robust Pt/Ru-codoped spinel cobalt oxide (PtRu-Co

Language: Английский

Citations

22
High-entropy alloy electrocatalysts go to (sub-)nanoscale DOI Creative Commons
Menggang Li,

Fangxu Lin,

Shipeng Zhang

et al.

Science Advances, Journal Year: 2024, Volume and Issue: 10(23)

Published: June 5, 2024

Alloying has proven power to upgrade metallic electrocatalysts, while the traditional alloys encounter limitation for optimizing electronic structures of surface sites in a continuous manner. High-entropy (HEAs) overcome this by manageably tuning adsorption/desorption energies reaction intermediates. Recently, marriage nanotechnology and HEAs made considerable progresses renewable energy technologies, showing two important trends size diminishment multidimensionality. This review is dedicated summarizing recent advances that are rationally designed electrocatalysis. We first explain advantages as electrocatalysts from three aspects: high entropy, nanometer, multidimension. Then, several structural regulation methods proposed promote electrocatalysis HEAs, involving thermodynamically nonequilibrium synthesis, regulating (sub-)nanosize anisotropic morphologies, well engineering atomic ordering. The general relationship between electrocatalytic properties further discussed. Finally, we outline remaining challenges field, aiming inspire more sophisticated HEA-based nanocatalysts.

Language: Английский

Citations

21
Methanol-Enhanced Low-Cell-Voltage Hydrogen Generation at Industrial-Grade Current Density by Triadic Active Sites of Pt1–Pdn–(Ni,Co)(OH)x DOI
An Pei,

Ruikuan Xie,

Lihua Zhu

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 13, 2025

Methanol (ME) is a liquid hydrogen carrier, ideal for on-site-on-demand H2 generation, avoiding its costly and risky distribution issues, but this "ME-to-H2" electric conversion suffers from high voltage (energy consumption) competitive oxygen evolution reaction. Herein, we demonstrate that synergistic cofunctional Pt1Pdn/(Ni,Co)(OH)x catalyst with Pt single atoms (Pt1) Pd nanoclusters (Pdn) anchored on OH-vacancy(VOH)-rich (Ni,Co)(OH)x nanoparticles create triadic active sites, allowing methanol-enhanced low-voltage generation. For MOR, OH* preferentially adsorbed Pdn then interacts the intermediates (such as *CHO or *CHOOH) favorably neighboring Pt1 assistance of bonding surface (Ni,Co)(OH)x. The enhanced selectivity *CHOOH pathway, instead *CO, sustains MOR activity to practically current density. HER, Pt1, Pdn, OH-vacancy sites an "acid–base" microenvironment facilitate water adsorption splitting, forming H* species *OH at vacancy, promote efficient asymmetric via Tafel mechanism. triadic-site synergy opens new avenues design synthesis highly stable catalysts "on-site-on-demand" production, here facilitated by methanol.

Language: Английский

Citations

11