Coordination number regulation of molybdenum single-atom nanozyme peroxidase-like specificity

Alkaline water splitting, especially anion-exchange-membrane based water electrolysis, is an attractive way for low-cost and scalable H2 production. Green electricity-driven alkaline water electrolysis requires that highly-efficient electrocatalysts be developed to further decrease the barriers of two half reactions – the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Various strategies have been exploited to date, among which atomic heterointerface engineering is the most promising strategy to overcome the intrinsic activity limitation of electrocatalysts. In this review, we thoroughly summarize the recent progress of atomic heterointerface engineering to improve the activity of electrocatalysts. The origin and rationale of the sluggish kinetics of the alkaline HER and OER are first introduced. Subsequently, the synergistic effects (ensemble effect and electron effect) of atomic heterointerface engineering to overcome the activity limitation are elaborated, in which the ensemble effect is helpful in optimizing the reaction pathways with enhanced reaction kinetics by creating a favorable heterointerface and the electron effect can balance the adsorption energies of reaction intermediates by coupling their electronic configurations. And then the rational design of the targeted electrocatalysts is concluded based on the heterointerface constituents and characteristics. At the end, some outlooks about the future development direction for optimizing and maximizing the interfacial active sites in the electrocatalysts are proposed.

Atomic heterointerface engineering overcomes the activity limitation of electrocatalysts and promises highly-efficient alkaline water splitting

The excessive dependence on fossil fuels contributes to the majority of CO2 emissions, influencing on the climate change. One promising alternative to fossil fuels is green hydrogen, which can be produced through water electrolysis from renewable electricity. However, the variety and complexity of hydrogen evolution electrocatalysts currently studied increases the difficulty in the integration of catalytic theory, catalyst design and preparation, and characterization methods. Herein, this review first highlights design principles for hydrogen evolution reaction (HER) electrocatalysts, presenting the thermodynamics, kinetics, and related electronic and structural descriptors for HER. Second, the reasonable design, preparation, mechanistic understanding, and performance enhancement of electrocatalysts are deeply discussed based on intrinsic and extrinsic effects. Third, recent advancements in the electrocatalytic water splitting technology are further discussed briefly. Finally, the challenges and perspectives of the development of highly efficient hydrogen evolution electrocatalysts for water splitting are proposed.

Rational Design of Better Hydrogen Evolution Electrocatalysts for Water Splitting: A Review

Although it is commonly believed that the water-dissociation-related Volmer process is the rate-limiting step for alkaline hydrogen evolution reaction (HER) on Pt-based catalysts, the underlying essence, particularly on the atomic scale, still remains unclear. Herein, it is revealed that the sluggish water-dissociation behavior probably stems from unfavorable orbital orientation and the kinetic issue is successfully resolved via N-induced orbital tuning. Impressively, N modified Pt-Ni nanowires deliver an ultralow overpotential of 13 mV at 10 mA cm-2 , which represents a new benchmark for alkaline HER catalysis. Fine-structural characterization and density functional theory analysis illustrate that the introduced nitrogen can uniquely modulate the electron densities around the Ni sites, and further create empty dz 2 orbitals with superior orientation for water adsorption and activation. More importantly, it is demonstrated that N-induced orbital modulation can generally boost the alkaline HER activities of Pt-Co, Pt-Ni, and Pt-Cu, offering a new perspective for the design of HER catalysts and beyond.

Boosting Water Dissociation Kinetics on Pt–Ni Nanowires by N-Induced Orbital Tuning

Semiconductor photocatalytic technology holds immense promise for converting sustainable solar energy into chemically storable energy, with significant applications in the realms of energy and the environment. However, the inherent issue of rapid recombination of photogenerated electrons and holes hinders the performance of single photocatalysts. To overcome this challenge, the construction of two-dimensional (2D) S-scheme heterojunction photocatalysts has emerged as an effective strategy. The deliberate design of dimensionality ensures a substantial interfacial area, while the S-scheme charge transfer mechanism facilitates efficient charge separation and maximizes redox capabilities. This review commences with a fresh perspective on the charge transfer mechanism in S-scheme heterojunctions, followed by a comprehensive exploration of preparation methods and characterization techniques. Subsequently, the recent advancements in 2D S-scheme heterojunction photocatalysts are summarized. Notably, the mechanism behind activity enhancement is elucidated. Finally, the prospects for the development of 2D S-scheme photocatalysts are presented. This article is protected by copyright. All rights reserved.

Construction of Two-Dimensional S-scheme Heterojunction Photocatalyst.

Preventing the high carrier recombination rate of graphitized C3N4 (GCN) is an urgent problem to be solved for its application as a photocatalyst for hydrogen production. Here, we first rationally embed the benzene ring in GCN to modify the local symmetry without changing its long-order structure. Theoretical calculation predicts that this design can change the electronic structure and promote the effective charge transfer in GCN. The benzene ring embedded GCN is successfully prepared by copolymerization using dicyandiamide and terephthalonitrile as precursors. Photoluminescence (PL) and time-resolved transient PL (TRPL) spectra confirm that the electron transfer efficiency of the benzene ring embed GCN is greatly improved. This nanomaterial displays 10.8 times higher photocatalytic hydrogen production rate than that of pristine GCN with the apparent quantum yield of 11.3% at 400 nm and 9% at 420 nm. This work provides a novel strategy for designing high-efficiency two-dimensional (2D) photocatalytic materials for water splitting.

Asymmetric embedded benzene ring enhances charge transfer of carbon nitride for photocatalytic hydrogen generation

An anti-photocorrosive photoanode based on a CdS/Ni x S y @NF heterostructure for visible-light-driven water splitting

A plasmonic bimetallic nanostructure has attracted considerable attention as a promising catalyst for light-driven catalytic reactions. The stability and recovery of the catalysts are still key issues for sustainable development of green chemistry. In this work, we designed and implemented an Au/Pd heterojunction@mesoporous SiO2 yolk–shell nanostructure (Au/Pd@m-SiO2 yolk–shell NPs) for plasmon-enhanced photocatalysis. The heterojunction of Au/Pd enhances the separation of hot electrons and holes under visible light irradiation, and the mesoporous SiO2 shell protects the active Au/Pd NPs from aggregation. The Au/Pd@m-SiO2 yolk–shell NPs exhibit extremely high stability for the plasmon-enhanced catalytic reduction of p-nitrophenol (4-NP) under visible light irradiation. The merging of a plasmonic material and a yolk–shell nanostructure proposes a new way for designing catalysts with good stability and promising activity.

Highly stable Au/Pd@mesoporous SiO2 yolk–shell hetero-nanostructures for plasmon-enhanced visible light driven catalytic reactions

Nanoscale chemical heterogeneity enables the co-existence of opposing superhydrophobic and hygroscopic properties

Facile band alignment of C3N4/CdS/MoS2 sandwich hybrid for efficient charge separation and high photochemical performance under visible-light

Handle everyday research tasks with reliable, citation-backed results

Your personal Research Agent to handle research tasks with citation-backed results

Popular Tasks used by Researchers

How can I help with your research?

Meet SciSpace

Get more enhanced response by uploading the PDFs you want me to reference.

No relevant PDFs in your library

SciSpace is the AI research assistant for academics. Run systematic literature reviews on 280M+ papers, and write papers with cited sources. Trusted by 1M+ students, PhDs & researchers.

SciSpace | AI for Research

Analyze PDFs

Code & Manuscripts

Funding & Grants

Literature & Patents

Medical & Clinical Data

Systematic Review

Visualize & Present

Web & Data

Build a Google Scholar-like website for your research.

Build a website

Create charts and images for your research

Create a Chart

Write a paper for submission to a journal

Draft a manuscript

Patent Search

Design eye-catching scientific posters in minutes.

Scientific Poster Generation

Systematic Literature Review

One task is running at the moment. Your messages will be shown right after.

Drag and drop or click here to browse

Loved by <highlight>1 million+</highlight> researchers

Extract a list of specific topics and their sources from unstructured text

Topics

Compare and analyze relevant papers that matches with your search

Papers

Get insights from PDFs and bookmarked papers from your library

My library

Recent searches

Try searching for:

Catch AI-generated content in scholarly and non-scholarly content

{ai} Detector

Ai Writer

Get PDF Summaries, highlighted text explanations 

Chat with PDF

Effortlessly create in-text citations and bibliographies in APA and 2,500 other formats

Citation generator

Get explanations, summaries, and answers on academic papers

Ease up your research workflow with {scispace}'s cohort of exciting AI tools

Elevate your academic writing skills and convey your ideas the way you want

Paraphraser

Explore our range of reading and writing tools

Your file is being prepared and should be ready in a few minutes. If it's a large file, it might take a bit longer. You can close this window, and we'll email you the file when it's done.

You have reached a maximum limit of <strong>{limit}</strong> columns in the table. Remove at least <strong>1</strong> column to add or create another one.

Haiyan Zhang

Author Tools

Chat about Author