Shiguo Zhang

• Doctor
• Professor (Full) at Hunan University

Electrosynthesis of high‐purity carbon monoxide (CO) from captured carbon dioxide (CO2) remains energy‐intensive due to the unavoidable CO2 regeneration and post‐purification stages. Here, we propose a direct high‐purity CO electrosynthesis strategy employing an innovative electrolyte, termed porous electrolyte (PE), based on “porous water”. Zeolit...

Electrosynthesis of high‐purity carbon monoxide (CO) from captured carbon dioxide (CO₂) remains energy‐intensive due to the unavoidable CO₂ regeneration and post‐purification stages. Here, we propose a direct high‐purity CO electrosynthesis strategy employing an innovative electrolyte, termed porous electrolyte (PE), based on "porous water". Zeolit...

Ionogels are a promising solution to improve the functionality of electrochromic devices (ECDs) by solving issues related to traditional liquid electrolytes, such as volatility, toxicity, and leakage. However, manufacturing ionogels...

Conjugated polymers containing donor (D) and acceptor (A) units possess intramolecular charge transfer (ICT) and typically exhibit lower bandgaps, facilitating a shift of the absorption peaks toward the red or...

Black-to-transmissive electrochromic (EC) materials, possessing superior electrochromic properties, still face limitations in smart windows, military camouflage, etc, due to their narrow spectrum modulation (below 800nm). In this work, strong acceptor...

Integrating anodic biomass valorization with carbon dioxide electroreduction (CO2RR) can produce value‐added chemicals on both the cathode and anode; however, anodic oxidation still suffers from high overpotential. Herein, a photothermal‐assisted method was developed to reduce the potential of 5‐hydroxymethyl furfural (HMF) electrooxidation. Capita...

High-purity ethylene production from CO2 electroreduction (CO2RR) is a coveted, yet arduous feat because the product stream comprises a blend of unreacted CO2, H2, and other off-target CO2 reduction products. Here we present an indirect reduction strategy for CO2-to-ethylene conversion, one that employs 2-bromoethanol (Br-EO) as a mediator. Br-EO i...

Both the sluggish sulfur redox reaction (SRR) kinetics and lithium polysulfides (LiPSs) shuttle effect limit the practical application of Li‐S batteries. Designing heterostructure sulfur hosts has emerged as an effective way to address these two issues with one material. However, the principles of heterostructures reinforced Li‐S batteries remain i...

The resistance of adhesives to organic solvents is of paramount importance in diverse industries. Unfortunately, many currently available adhesives exhibit either weak intermolecular chain interactions, resulting in insufficient resistance to organic solvents, or possess a permanent covalent crosslinked network, impeding recyclability. This study i...

The advancement of contemporary adhesives is often limited by the balancing act between cohesion and interfacial adhesion strength. This study explores an approach to overcome this trade-off by utilizing the spontaneous polymerization of a protic ionic liquid-based monomer obtained through the neutralization of 2-acrylamide-2-methyl propane sulfoni...

Electrochromic devices built with ionogel electrolytes are seen as a pivotal step towards the future of quasi‐solid electrochromic devices, due to their striking properties like exceptional safety and high ionic conductivity. Yet, the poor mechanical strength of electrolyte of these devices remains a constraint that hampers their advancement. As a...

In this study, Co/Ni‐NC catalyst with hetero‐diatomic Co/Ni active sites dispersed on nitrogen‐doped carbon matrix is synthesized via the controlled pyrolysis of ZIF‐8 containing Co²⁺ and Ni²⁺ compounds. Experimental characterizations and theoretical calculations reveal that Co and Ni are atomically and uniformly dispersed in pairs of CoN4‐NiN4 wit...

Pervasive intrinsic defects have a significant impact on the electrocatalytic activity of carbon materials, but previous research has focused on the effects of topological structures exclusively. Herein, a compelling demonstration of the pivotal role played by the positions and spatial arrangement of intrinsic defects in determining their efficacy...

Electrocatalyst is commonly regarded as the primary source of activity in electrochemical reactions, while the other modules of catalysis electrode, such as the current collector, are typically assumed to be...

Single-atom, confined in crystalline porous materials such as metal-organic framework (MOF), features unparalleled multidimensional interactions with the molecular wall of the nano-cavity, showcasing a synergistic catalytic effect. Nevertheless, the insulating...

Increasing the liquid content has been recognized as an effective strategy to enhance the Li+ conductivity and electrode compatibility of gel electrolytes for lithium-metal batteries (LMBs). However, a low gelator...

Transforming wastes or hazardous materials into value-added chemical products is of great concern from economic , environmental, and sustainable prospects. Various approaches were implemented to convert CO 2 into valuable/fine chemicals, e.g., chemical fixation, electro-, thermal-, and photo-catalysis. The electrochemical reduction pathway of CO 2...

The local microenvironment of single-atom electrocatalysts (SACs) governs their activity and selectivity. While previous studies have focused on the first coordination shell (FCS) of metal centers, functional species beyond FCS...

Ionogels for lithium metal batteries are usually obtained by immobilization of lithium salt-containing ionic liquids using linear polymers as gelator, which are thermally unstable and lack of adhesion. Meanwhile, the two-cation (ionic liquid cation and lithium ion) competition results in low lithium-ion transference number. In this work, we designe...

Graphite can be successfully used as an anode for potassium-ion batteries (PIBs), while its conversion to KC8 leads to huge volume expansion, destruction of solid electrolyte interphase (SEI), and thus poor cycling stability. Incorporating additives into electrolytes is an economical and effective way to construct robust SEI for high-performance PI...

Low-molecular-weight adhesives (LMWAs) possess many unique features compared to polymer adhesives. However, fabricating LMWAs with adhesion strengths higher than those of polymeric materials is a significant challenge, mainly because of the relatively weak and unbalanced cohesion and interfacial adhesion. Herein, an ionic liquid (IL)-based adhesive...

Solid‐state Li batteries are receiving increasing attention as a prospective energy storage system due to the high energy density and improved safety. However, the high interfacial resistance between solid‐state electrolyte and electrode results in sluggish Li⁺ transport kinetics. To tackle the interfacial problem and prolong the cycle life of soli...

Lithium-sulfur (Li-S) batteries have been considered as a promising candidate for next-generation energy storage, yet their practical application is limited by the polysulfides (PS) shuttle effect and slow kinetics of sulfur redox reaction. Despite the progress in engineering the separator for Li-S batteries, the separator with the synergistic effe...

Developing suitable anode materials for potassium-ion batteries (PIBs) remains a great challenge owing to the limited theoretical capacity of active materials and large radius of K⁺ ion (1.38 Å). To solve these obstacles, by integrating the principles of multielectron transfer and rational porous crystal framework, we creatively propose the monocli...

Although tremendous efforts have been made to remedy the dissolution of lithium polysulfide (LiPS) intermediates in Li-S batteries, the sluggish sulfur reduction reaction (SRR) are still less addressed. Here, we...

Molecular catalysts are acknowledged for the ability to design reaction sites within well‐defined structures to achieve high catalytic activities. However, in many cases, molecular catalysts undergo structural changes to some other form(s), which are finally the real catalysts. Here, we report two half‐sandwich ruthenium complexes; [Ru([9]aneN3)(bp...

Adhesive materials have wide applications in diverse fields, but the development of a novel and multipurpose adhesive is a great challenge. This study demonstrates that conventional poly(ionic liquid)s (PILs) can be designed as highly efficient adhesives by simply introducing alkoxy moieties into the cationic backbone of PILs containing bis(trifluo...

Two-dimensional (2D) coordination polymers are very interesting materials for their attractive applications. A novel 2D metal-organic framework (MOF) was derived from copper(II) and amino benzoic acid under both room temperature and solvothermal reaction conditions using different solvents. From both synthesis methods, an identical MOF was crystali...

A Au-doped SrTiO3perovskite oxide catalyst (Sr0.995Au0.005TiO3−δ) has been designed and synthesized based on thermodynamic analysis and density functional theory calculations. During reduction, Au nanoparticles with an average diameter of 2 nm arein situexsolved and evenly distributed on the surface of a SrTiO3substrate. The as-prepared catalyst sh...

Replacing conventional metal-N4 moieties with different coordination structures is a promising strategy to tailor the activity and selectivity of single-atom catalysts (SACs). However, for CO2 electroreduction driven by metals that may produce diverse chemical species, such as Tin (Sn), the influences of nonnitrogen coordination environments on the...

Lithium-sulfur (Li-S) battery with high theoretical energy density has been considered as an important energy storage system. However, its application has been limited by low cycling stability and rapid capacity decay due to the shuttle of lithium polysulfide (Li2Sn, n > 5). These problems can be solved using small sulfur molecules (S2–4) as the ac...

Dual single-cobalt atom-based catalysts were synthesized using CoN3 sites and N dopants co-decorated hierarchically porous carbon (HPC-Co) as the matrix to immobilize cobalt phthalocyanine (CoPc). CoPc interacts with N dopants and CoN3, forming N-CoPc and CoN3-CoPc sites via π–π and Co-Co interactions. HPC-Co/CoPc (5:1) produced syngas at industria...

Nonaqueous potassium-ion batteries (KIBs) have been regarded as a promising alternative energy system to lithium-ion batteries, due to the abundance of the K resource and unique electrochemical properties. However, exploring suitable KIB cathode materials remains a great challenge, owing to the much larger size of the K ion than that of the Li ion....

Water purification is an important issue in our daily life. Various pollutants, from micrometer-sized microorganisms to molecular- or atomic-sized pollutants, need to be efficiently removed from water. Unlike traditional cascade-stage techniques, we report a one-step water purification method based on a ceramic aerogel composed of porous BN fibers,...

Binders as a necessary component in sulfur cathodes play an important role in maintaining the mechanical integrity/stability of electrode and anchoring lithium polysulfide (LiPS) for Lithium-sulfur (Li-S) batteries. In this work, we developed a low-cost and water-soluble polyelectrolyte binder (D-PAA/C-EA) by simply neutralizing commercially availa...

Manipulating the in‐plane defects of metal–nitrogen–carbon catalysts to regulate the electroreduction reaction of CO2 (CO2RR) remains a challenging task. Here, it is demonstrated that the activity of the intrinsic carbon defects can be dramatically improved through coupling with single‐atom Fe–N4 sites. The resulting catalyst delivers a maximum CO...

The lithium-sulfur battery (Li–S) is a promising energy storage system with many advantages over the commercialized lithium-ion battery. It has a high theoretical capacity of 1675 mAh g⁻¹, a high theoretical energy density (2600 Wh kg⁻¹), and is eco-environmentally friendly. Although only a small amount is used (<10 wt%) in the electrode, binders m...

Perovskite oxides have been intensively studied for electrochemical catalysis, due to their tunable composition, low cost, and strong structure-activity relationship. Here we report a novel and facile strategy to enhance the ORR activity and stability of Ba0.5Sr0.5Co0.8Fe0.2O3-δ (BSCF) perovskite oxide through engineering the surface electronic str...

Heteroatom-doped meso/micro-porous carbon materials are conventionally produced by harsh carbonization under an inert atmosphere involving specific precursors, hard/soft templates, and heteroatom-containing agents. Herein, we report a facile synthesis of N and O co-doped meso/micro-porous carbon (NOMC) by template-free carbonization of a small-mole...

The sluggish kinetics of the oxygen evolution reaction (OER) at the anode severely limit hydrogen production at the cathode in water splitting systems. Although electrocatalytic systems based on cheap and earth‐abundant copper catalysts have shown promise for water oxidation under basic conditions, only very few examples with high overpotential can...

Anion exchange membrane fuel cells (AEMFCs) have drawn great attention since the alkaline condition enables the use of non-platinum catalysts. Nevertheless, the lack of alkali-stable and highly conductive anion exchange membranes (AEMs) impedes the development of AEMFCs. Herein, a series of novel quaternized Tröger's base polymer AEMs are prepared...

Platinum is generally known as the most effective electrocatalyst for hydrogen evolution reaction because it can greatly lower the overpotential and accelerate the reaction kinetics, while its commercial potential always suffers from scarcity, high cost, low utilization, and poor durability particularly in acidic electrolytes. We herein demonstrate...

Although some ligand transformations involved in metal complexes have been reported during water oxidation (WO) ((photo)chemical/electrochemical), such as ligand decomposition, partial oxidation, or complete dissociation, however, ligand photodissociation has not been reported yet. Here, we report the first example of ligand photodissociation in [R...

Nitrogen-doped porous carbon materials (NPCMs) are usually obtained by carbonization of complicated nitrogen-containing polymers in the presence of template or physical/chemical activation of the as-synthesized carbon materials. Herein we reported the facile synthesis of NPCMs by direct carbonization of a series of furfuryl amine (FA)-based protic...

Embedding the fragmented selenium into the micropores of carbon host has been regarded as an effective strategy to change the Li–Se chemistry by a solid–solid mechanism, thereby enabling an excellent cycling stability in Li–Se batteries using carbonate electrolyte. However, the effect of spatial confinement by micropores in the electrochemical beha...

Highly efficient electrocatalysts towards hydrogen evolution reaction (HER) with large current density at all-pH values are critical for the sustainable hydrogen production. Herein, we report a free-standing HER electrode, phosphorous-doped molybdenum nitride nanoparticles embedded in 3-dimentional carbon nanosheet matrix (P-Mo2N-CNS) fabricated vi...

Designing a low-cost, high-efficiency and robust doped-carbon-based oxygen reduction reaction electrocatalyst for large-scale implementations of fuel cells is highly desirable but challenging. In this work, we report a new type of hollow Fe3O4 with oxygen vacancy incorporating on mesoporous carbon prepared by pyrolyzing mesoporous carbon enriched w...

The development of both H2–O2 proton exchange membrane fuel cells (PEMFCs) and Zn-air batteries are challenged by high-efficiency air cathodes with a high oxygen reduction reaction (ORR) electrocatalytic-activity. The increase of density and accessibility of active sites are widely accepted effective approach to boost the oxygen reduction reaction....

Atomically dispersed Fe–N–C catalysts with additional Fe-containing nanoparticles including metal, carbides or oxides have shown great potentials towards oxygen reduction reaction (ORR) catalysis. However, the formation of these synergistically active nanoparticles and the effect of the porous carbon structures remain unclear. In this work, a novel...

Highly efficient and cost-effective electrocatalysts towards both oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are critical for the large-scale and environmental-friendly hydrogen production. Here we report the facile synthesis of a novel bifunctional catalyst, mesoporous Co3O4 with surface decorated epitaxial S-doped CoO l...

Highly water-soluble cyanocobalamin (also known as vitamin B12) is the most structurally macrocyclic complex comprising cobalt in the center of a corrin ring. Interestingly, it acts as a robust electrocatalyst in water oxidation at ∼0.58 V overpotential with a Faradaic efficiency of 97.50% under the neutral buffered conditions. The catalyst is impr...

Towards practical lithium-sulfur batteries, the rational design of sulfur host that enables highly efficient sulfur electrochemistry and high areal sulfur loading is essential but still a challenge. Here, a class of 3D nanocomposite architecture featured by necklace-like structure contains intertwined carbon-nanotubes (CNTs) and defective Prussian...

Carbon-based electrocatalysts with single-metal-site hold great potential for the mechanism exploration via mimicking molecular catalysts, due to their distinct catalytic sites. In addition to metal atoms, the neighboring non-metal heteroatoms such as N, S, and O atoms, which are widely detected in carbon-based single-atom catalysts, may also contr...

Highly active and stable catalysts towards electrochemical oxygen evolution reaction are crucial for the efficient water splitting and sustainable hydrogen generation. Here we report a novel mesoporous Co3O4 with the surface decoration of mixed CoOxPy species towards efficient OER catalysis. The material is synthesized from a simple carbon template...

In this study, a new DMF-derived ionic liquid electrolyte [EDMF]BF4 was prepared, characterized and applied as a high-capacitance electrolyte for electric double-layer capacitors (EDLCs). [EDMF]BF4 was measured to have very high ionic conductivity and low viscosity (24.8 mS cm⁻¹ and 21.6 mPa s at 25 °C), as well as a comparable electrochemical wind...

In this study, the anion exchange reaction of an organic cation chloride with excess KHCO2 to synthesize formate-based ionic liquids (ILs) was performed in water, and the water-miscible IL products were easily obtained via salting-out phase separation caused by the excess KHCO2. According to the synthesis results, a set of heuristic rules could be...

Although several Si/C composite structures have been proposed for high-performance lithium-ion batteries (LIBs), they have still suffered from expensive and complex processes of nano-Si production. Herein, a simple, controllable oxygen inward diffusion was utilized to transform Si sludge obtained from the photovoltaic (PV) industry into the nano-Si...

Protic ionic liquids/salts derived metal free and iron-doped carbon materials with tunable physic-chemical properties. Importance of N-content, the configuration of N, porosity, surface area, and Fe content on the electroreduction of oxygen in aqueous media.

Our previous study (J. Mater. Chem. A, 2018, 6, 3171-3180) theoretically predicted that the scandium oxide (ScO2) monolayer can deliver high specific capacity and energy density as the active material of the lithium-ion (Li-ion) battery, but the voltage will drop below 0.5 V when ScO2 is lithiated to LiScO2 during the discharge process. The current...

Using Li2S as an active material and designing nanostructured cathode hosts are considered as promising strategies to improve the performance of lithium-sulfur (Li-S) batteries. In this study, the reaction mechanisms during delithiation of nanoconfined Li2S as active material, represented by a Li20S10 cluster, are examined by first-principles based...

Electrode host materials play a critical role in determining the electrochemical performance of the energy storage devices such as alkali metal-ion batteries. Cathode host materials are expected to provide good electronic and ionic conductivity, improved specific capacity and high discharge voltage. Two-dimensional (2D) transition metal dichalcogen...

The major bottleneck for widespread realization of fuel cells has been the usage of precious-metal-based electrocatalysts, such as Pt/C or Pt-alloy/C, at the cathode. Owing to the high cost and limited natural resources of platinum, nonprecious metal catalysts, such as iron-doped carbons, have emerged as promising substitute catalyst materials. Pro...

Lithium–sulfur (Li–S) batteries have attracted interest as a promising energy-storage technology due to their overwhelming advantages such as high energy density and low cost. However, their commercial success is impeded by deterioration of sulfur utilization, significant capacity fade, and poor cycle life, which are principally originated from the...

The preparation of ionic liquids most often involves the use of organic solvents or hazardous chemicals, especially for hydrophilic ionic liquids prepared from metathesis reaction. In this study, the salting-out effect was proposed to promote the metathesis reaction to afford water-miscible ionic liquids. The reaction proceeds in aqueous solution s...

Ionic liquids (ILs) are liquids consisting entirely of ions and can be further defined as molten salts having melting points lower than 100 °C. One of the most important research areas for IL utilization is undoubtedly their energy application, especially for energy storage and conversion materials and devices, because there is a continuously incre...

Ionic liquids (ILs) have been widely investigated as novel solvents, electrolytes, and soft functional materials. Nevertheless, the widespread applications of ILs in most cases have been hampered by their liquid state. The confinement of ILs into nanoporous hosts is a simple but versatile strategy to overcome this problem. Nanoconfined ILs constitu...

Nitrogen/sulfur-codoped mesoporous carbon (CMK-3P) was readily prepared through direct carbonization of a protic salt [Phen][2HSO4] in the presence of pristine SBA-15 template without the use of acid or metal catalysts for prepolymerization. CMK-3P is characteristic of the presence of large mesopores and even macropores caused by the curved and int...

Fundamental Properties of Nitrogen Doped Carbon Materials from Protic Ionic Liquids/Salts and implications of the structural factors in CO2 Adsorption and Oxygen Reduction Reaction

Ether groups are well-known for their unique contribution to low viscosity and high conductivity, and hence ether-functionalized ionic liquids (ILs) have been widely studied and successfully employed in various applications. However, the ether chain length effect on physicochemical properties is complex and still lack of a systematic study. In this...

Lithium-sulfur (Li-S) batteries are a promising energy-storage technology owing to their high theoretical capacity and energy density. However, their practical application remains challenges because of the serve shuttle effect caused by the dissolution of polysulfides in common organic electrolytes. Polysulfide-insoluble electrolytes, such as solva...

Electrochemical energy systems such as fuel cells and metal–air batteries [1, 4] are based on oxygen reduction reaction (ORR) which is intrinsically sluggish in kinetics. So, the importance of efficient, low-cost and stable electrocatalysts for such systems is paramount. In this study, we prepared metal (Fe) and nitrogen (N) doped mesoporous carbon...

Lithium-ion sulfur batteries with a [graphite|solvate ionic liquid electrolyte|lithium sulfide (Li2S)] structure are developed to realize high performance batteries without the issue of lithium anode. Li2S has recently emerged as a promising cathode material, due to its high theoretical specific capacity of 1166 mAh/g and its great potential in the...

Instead of being seen as alternative solvents and electrolytes for organic reactions, catalysis, separation, electrochemistry, and so on, ionic liquids (ILs) consisting of discrete cations and anions have recently emerged as versatile building blocks for advanced functional materials. A number of functional ILs and IL-containing composite materials...

Salts that are liquid at room temperature, now commonly called ionic liquids, have been known for more than 100 years; however, their unique properties have only come to light in the past two decades. In this Review, we examine recent work in which the properties of ionic liquids have enabled important advances to be made in sustainable energy gene...

Solidification of fluidic ionic liquids into porous materials yields porous ionic networks that combine the unique characteristics of ionic liquids with the common features of polymers and porous materials. This minireview reports the most recent advances in the design of porous ionic liquids. A summary of the synthesis of ordered and disordered po...

Lithium sulfide (Li2S) as a cathodic material in Li–S batteries can not only deliver a high theoretical specific capacity of 1166 mAh/g, but also is essential for batteries using Li-free anode materials such as silicon and graphite. Various efforts have been made to synthesize a highly efficient Li2S–carbon composite; however, the electronically an...

Traditional methods of preparing highly porous, nitrogen/sulfur-codoped carbons require either template-based tedious, time-consuming procedures or harsh chemical/physical activation process. In this paper, we report a very facile method to prepare such carbons via the direct carbonization of a single protic salt, prop-2-en-1-aminium hydrogensulfat...

1. Introduction Lithium sulfide (Li 2 S) with a high theoretical specific capacity of 1166 mAh/g has recently been adopted as a promising cathode-active material for lithium batteries, because of its conjunction with safer lithium-free anodes. However, Li 2 S is electronically and ionically insulating in nature, and has a high melting point, which...

Solidification of fluidic ionic liquids into porous materials yields porous ionic networks that combine the unique characteristics of ionic liquids with the common features of polymers and porous materials. This minireview reports the most recent advances in the design of porous ionic liquids. A summary of the synthesis of ordered and disordered po...

Three-dimensionally macroporous nitrogen-doped carbon materials are fabricated via carbonization of an ionic-liquid-based small molecule precursor, 1-ethyl-3-methylimidazolium dicyanamide, using opal silica colloidal crystals as a hard template. As compared to traditional polymerizable monomer-based precursors such as furfuryl alcohol, the entire p...

Graphitic carbon nitride (g-C3N4) is traditionally obtained by thermal polycondensation of nitrogen-rich organic nonionic precursors. Herein, we provide a new and simple strategy for the synthesis of g-C3N4 through direct thermal condensation of single protic guanidine salts with various anions. The thermal condensation process, and the structure a...

Nitrogen/sulfur-co-doped mesoporous carbon (Phen-HS) was obtained through direct carbonization of a single protic salt, that is, 1,10-phenanthrolinium dibisulfate ([Phen][2 HSO4 ]), in the presence of a colloidal silica template without the use of additional acid or metal catalysts for prepolymerization prior to carbonization. Phen-HS was prepared...

The rapidly increasing demand for electrical and hybrid vehicles and stationary energy storage requires the development of “beyond Li-ion batteries” with high energy densities that exceed those of state-of-the-art Li-ion batteries. Li–S batteries, which have very high theoretical capacities and energy densities, are believed to be one of the most p...

Traditional methods for preparation of nitrogen-doped mesoporous carbons (NMCs), especially NMCs with high nitrogen content and narrow pore size distribution, typically require tedious, time-consuming procedures involving polymer precursors (or monomers for pre-polymerization), specific templates, and/or nitrogen-containing agents, as well as addit...

Nitrogen-doped carbon materials (NDCs) play an important role in various fields. A great deal of effort has been devoted to obtaining carbon materials with a high nitrogen content; however, much is still unknown about the structure of the nitrogen-doped materials and the maximum nitrogen content possible for such compounds. Here, we demonstrate an...

Nitrogen-doped carbon materials (NDCs) play an important role in various fields. A great deal of effort has been devoted to obtaining carbon materials with a high nitrogen content; however, much is still unknown about the structure of the nitrogen-doped materials and the maximum nitrogen content possible for such compounds. Here, we demonstrate an...