Hydrogen Intercalation‐Induced Crystallization of Ternary PdNiP Alloy Nanoparticles For Direct Formic Acid Fuel Cells DOI
Hongfei Cheng, Jun Zhou,

Huiqing Xie

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(14)

Published: Feb. 17, 2023

Abstract Direct formic acid fuel cells (DFAFCs) are among the promising energy sources in future low‐carbon economy. A key challenge hindering their scale‐up and commercialization is lack of efficient electrocatalysts for anodic oxidation (FAO). Very recently, FAO performance palladium hydrides (PdH x ) has been found to be superior pristine Pd that well known its high intrinsic activity. However, there enormous space controlled synthesis electrocatalytic behaviors PdH ‐based nanomaterials awaiting explored. Herein, hydrogen intercalation‐induced crystallization PdNiP alloy nanoparticles reported, obtained PdNiP‐H exhibit excellent performance. Of particular note, stability much better than Pd‐H. Furthermore, used as anode catalyst a prototype DFAFC, which demonstrate higher power density commercial Pd/C. Density functional theory calculations show synergistic effect alloying Ni P endows with preference toward via direct pathway anti‐CO* poisoning capability. This work shines new light on development nanoalloys good activity DFAFC applications.

Language: Английский

Reversible hydrogenation of carbon dioxide to formic acid using a Mn-pincer complex in the presence of lysine DOI Creative Commons
Duo Wei, Rui Sang, Peter Sponholz

et al.

Nature Energy, Journal Year: 2022, Volume and Issue: 7(5), P. 438 - 447

Published: May 19, 2022

Abstract Efficient hydrogen storage and release are essential for effective use of as an energy carrier. In principle, formic acid could be used a convenient medium via reversible CO 2 hydrogenation. However, noble metal-based catalysts currently needed to facilitate the (de)hydrogenation, produced during is generally released, resulting in undesirable emissions. Here we report α -amino acid-promoted system hydrogenation using Mn-pincer complex homogeneous catalyst. We observe good stability reusability catalyst lysine amino at high productivities (CO hydrogenation: total turnover number 2,000,000; dehydrogenation: 600,000). Employing potassium lysinate, achieve >80% H evolution efficiency >99.9% retention ten charge–discharge cycles, avoiding re-loading steps between each cycle. This process was scaled up by factor 18 without obvious drop productivity.

Language: Английский

Citations

182
Formic Acid to Power towards Low‐Carbon Economy DOI
Indranil Dutta, Sudipta Chatterjee, Hongfei Cheng

et al.

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(15)

Published: Feb. 23, 2022

Abstract The storage and utilization of low‐carbon electricity decarbonization transportation are essential components for the future energy transition into a economy. While hydrogen has been identified as potential carrier, lack viable technologies safe efficient H 2 greatly limits its applications deployment at scale. Formic acid (FA) is considered one promising carriers because high volumetric capacity 53 g /L, relatively low toxicity flammability convenient low‐cost transportation. FA can be employed to generate either in direct fuel cells (FCs) or indirectly an source FCs. enable large‐scale chemical eliminate energy‐intensive expensive processes liquefaction compression thus achieve higher efficiency broader utilization. This perspective summarizes recent advances catalyst development selective dehydrogenation high‐pressure production. advantages limitations FA‐to‐power options highlighted. Existing life cycle assessment (LCA) economic analysis studies reviewed discuss feasibility fuel.

Language: Английский

Citations

165
Electroreduction of CO2: Advances in the Continuous Production of Formic Acid and Formate DOI Creative Commons

Kevin Fernández-Caso,

Guillermo Díaz‐Sainz, Manuel Álvarez-Guerra

et al.

ACS Energy Letters, Journal Year: 2023, Volume and Issue: 8(4), P. 1992 - 2024

Published: March 30, 2023

The study of the electrochemical CO2 reduction to obtain formate (HCOO–) or formic acid (HCOOH) is receiving much attention as a promising technology. Since continuous–mode operation has become necessary for practical implementation reduction, recent years have seen rapid increase in number research approaches focusing on this aspect. This Focus Review provides unified discussion available studies continuous electroreduction HCOO–/HCOOH, considering different important features process design. Moreover, paper quantitatively assesses performance that involve reactors converting HCOOH/HCOO–, comparing relevant typically used figures merit, including energy consumption. Although some trade-offs already been achieved, simultaneous optimization all merit remains challenge. Finally, concluding remarks highlight detected trends and discuss aspects will be tackled by future field.

Language: Английский

Citations

165
Tunable Selectivity for Electrochemical CO2 Reduction by Bimetallic Cu–Sn Catalysts: Elucidating the Roles of Cu and Sn DOI
Maolin Zhang, Zedong Zhang, Zhenghang Zhao

et al.

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(17), P. 11103 - 11108

Published: Aug. 20, 2021

Production of formate or CO from electrochemical CO2 reduction reactions (eCO2RRs) represents a promising way to utilize with future low-carbon electricity produce value-added chemicals and fuels. Herein, series Cu–Sn composite catalysts were designed for eCO2RRs. The products could be tuned selectively by varying the Cu/Sn composition. catalyst Cu1Sn1 CuSn alloy core SnO shell structure doped small amount Cu gives maximum faradic efficiency (FE) 95.4 at −1.2 V. In contrast, single-Sn-atom-doped Cu20Sn1 is selective FE 95.3% −1.0 DFT results reveal that existence amounts Sn single atoms in these two critical reducing reaction free energies reduction, resulting formation CO, respectively.

Language: Английский

Citations

129
Continuous electroproduction of formate via CO2 reduction on local symmetry-broken single-atom catalysts DOI Creative Commons
Juncai Dong, Yangyang Liu, Jiajing Pei

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Oct. 27, 2023

Abstract Atomic-level coordination engineering is an efficient strategy for tuning the catalytic performance of single-atom catalysts (SACs). However, their rational design has so far been plagued by lack a universal correlation between symmetry and properties. Herein, we synthesised planar-symmetry-broken CuN 3 (PSB-CuN ) SACs through microwave heating electrocatalytic CO 2 reduction. Remarkably, as-prepared exhibited selectivity 94.3% towards formate at −0.73 V vs. RHE, surpassing symmetrical 4 catalyst (72.4% −0.93 RHE). In flow cell equipped with PSB-CuN electrode, over 90% was maintained average current density 94.4 mA cm −2 during 100 h operation. By combining definitive structural identification operando X-ray spectroscopy theoretical calculations, revealed that intrinsic local breaking from planar D configuration induces unconventional dsp hybridisation, thus strong activity microenvironment metal centre (i.e., number distortion), high preference production in moiety. The finding opens avenue designing specific symmetries selective electrocatalysis.

Language: Английский

Citations

116
A Nanocomposite of Bismuth Clusters and Bi2O2CO3 Sheets for Highly Efficient Electrocatalytic Reduction of CO2 to Formate DOI
Lin Li, Xiaoyang He, Xia‐Guang Zhang

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(3)

Published: Oct. 29, 2022

The renewable-electricity-driven CO2 reduction to formic acid would contribute establishing a carbon-neutral society. current catalyst suffers from limited activity and stability under high selectivity the ambiguous nature of active sites. Herein, we report powerful Bi2 S3 -derived that demonstrates density 2.0 A cm-2 with formate Faradaic efficiency 93 % at -0.95 V versus reversible hydrogen electrode. energy conversion single-pass yield reach 80 67 %, respectively, durability reaches 100 h an industrial-relevant density. Pure concentration 3.5 mol L-1 has been produced continuously. Our operando spectroscopic theoretical studies reveal dynamic evolution into nanocomposite composed Bi0 clusters O2 CO3 nanosheets pivotal role -Bi2 interface in activation conversion.

Language: Английский

Citations

110
Metal-organic framework derived dual-metal sites for electroreduction of carbon dioxide to HCOOH DOI
Kaili Yao, Haibin Wang, Xiaotao Yang

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 311, P. 121377 - 121377

Published: April 7, 2022

Language: Английский

Citations

72
Efficient Conversion of Biomass to Formic Acid Coupled with Low Energy Consumption Hydrogen Production from Water Electrolysis DOI Open Access
Wensi Tang, Lunan Zhang, Tianyu Qiu

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(30)

Published: May 26, 2023

The development of a new electrolytic water hydrogen production coupling system is the key to realize efficient and low-cost promote its practical application. Herein, green electrocatalytic biomass formic acid (FA) coupled has been developed. In such system, carbohydrates as glucose are oxidized FA using polyoxometalates (POMs) redox anolyte, while H2 evolved continuously at cathode. Among them, yield high 62.5 %, only liquid product. Furthermore, requires 1.22 V drive current density 50 mA cm-2 , Faraday efficiency close 100 %. Its electrical consumption 2.9 kWh Nm-3 (H2 ), which 69 % that traditional water. This work opens up promising direction for with conversion.

Language: Английский

Citations

59
Recent advances of single-atom alloy catalyst: Properties, synthetic methods and electrocatalytic applications DOI Creative Commons
Jiahao Zhuang, Dingsheng Wang

Materials Today Catalysis, Journal Year: 2023, Volume and Issue: 2, P. 100009 - 100009

Published: June 27, 2023

Developing high-performance and cost-effective electrocatalysts for clean renewable energy conversion process has been proved a promising approach to deal with the global environment issues. Single-atom alloy (SAA) catalyst, foreign metal atoms atomically dispersed in surface of host metal, combines merits conventional alloys single-atom catalysts. The maximum atomic utilization active unique structural electrical properties SAA offer great potential boosting electrocatalytic activity reducing cost manufacture. Meanwhile, well-defined sites raise an opportunity shed light on structure-activity relationship further direct synthesis high-efficiency electrocatalysts. Herein, we focus recent developments advanced catalysts discussed general SAAs. Then design principle synthetic methods were summarized. Next, highlighted practical applications SAAs chemicals production, including hydrogen evolution reaction, oxygen CO2 reduction N2 reaction other representative reactions. Finally, challenges future directions are presented.

Language: Английский

Citations

57
Upcycling of non-biodegradable plastics by base metal photocatalysis DOI Creative Commons
Chenfei Li, Xin Ying Kong,

Maoping Lyu

et al.

Chem, Journal Year: 2023, Volume and Issue: 9(9), P. 2683 - 2700

Published: Aug. 14, 2023

Language: Английский

Citations

51